There are a number of things that will effect your speed here. How the other machines access the files on your HTPC is one of them. Transcoding and file serving are very different things and file serving is much less taxing on your CPU. You should be able to gauge a rough idea of your bottleneck in Task Manager by pressing ctrl+alt+del and looking at the Resource Monitor while your users are connected. Your method of connecting may also be a factor, ie a network connector with low data throughput will easily become saturated with multiple users and large media files. RAM is also a factor, as well as the speed of your disks and the number of processes that you have running at any one time. If you have a 2nd SSD for programs and user folders I assume that you use the term HTPC loosely - my HTPC has Win7, XBMC, utorrent, itunes and firefox on its 60GB SSD and is not even close to full...
And no, caching your 9TB E: drive onto an SSD will probably not help you at all. If you have massive directories, try breaking them down into folders. SSD caching is designed to speed up a system by indexing the contents of a larger spindle drive (basically). It works by storing information about regularly accessed files ect. Unless your three users enjoy watching the same thing over and over again, I can't see how it would help. It sounds like what you are trying to do is make one 9TB hybrid drive, which firstly I don't think is possible and secondly would require quite a lot of SSD cache space to be effective (in any usage).
A faster RAID array would be RAID1+0 or RAID0+1 but then I have to ask, why bother with RAID? I used to use RAID arrays, mostly because I didn't know much about them and I knew servers used them, so I assumed that they were desirable in my system. RAID arrays are designed to offer redundancy, that is to say, to offer some kind of protection against actual hardware failure. In a commercial application, where servers work 24/7, this can become a real issue. When a hard disk physically fails you need to be able to replace that drive and get the server back online and back to work. RAID (note the "R") is the perfect way to offer this kind of redundancy. For domestic applications where you have one or more users who tend not to know a great deal about computers and who therefor often make mistakes or don't follow proper proceedures, the biggest problem tends to be data protection - we don't want to lose our stuff. The best solution for this problem is backing up data. That is not what RAID is designed for. There are software applications that are designed to back up data but I personally find them to be gimmicky and a waste of space. They exist because some people enjoy them but I personally would rather do it manually. I don't advocate USB hard drive backups because people tend to move external drives while they are on and this greatly reduces the life expectancy of any platter drive. I simply have internal drives that I back my data up onto manually and that I don't share over the network. At first glance this may seem like like doing RAID1 the hard way but there are two major differences - firstly RAID1 is slower that one disk when it comes to retrieving my data and secondly RAID1 doesn't duplicate my data files onto another disk, it mirrors the ENTIRE disk. What that means is that of your file system becomes corrupt, or you get a bad cluster one one disk, or a virus or something, it will copy that error onto the second disk. You don't get to go back in time, you don't get to switch it up - you just end up with two sick disks instead of one. It doesn't matter if you're honest john backing up your personal camcorder videos or mr antiestablishment illegally downloading everything you can get your hands on - if one drive fails and you lose a handfull of files that you haven't backed up yet, it's a damn sight less annoying that losing your entire disk. Not to mention that you probably paid a pretty penny for your 4th 3TB drive, that you can't even see in RAID5.
In my own personal opinion ( I won't pretend to be humble as I wander the internet voicing my views) You should check your resource monitor and look for a bottleneck. You should also get to thinking about whether or not you need your RAID array or if hosting your files in well seperated folders on different drives in your computer may be of more real life benifit. Sure it is isn't risk free but then again, if one of your RAID drives does fail you're immediately at risk of losing the entire array - not only until you replace the drive but until the replacement drive has been populated with all of the data that is required of it to work as a member of your array. RAIDing your system can become quite an expensive hobby in this way and I think that many people are greatly confused about the benefits that they think they are gaining. All you are doing is protecting yourself against disk hardware failure, at the expense of speed and the cost of hard drives. The best possible solution for protecting your data, is backing it up. You can even use other forms of media to do this, you don't have to spend hundreds of dollars on hard disks...
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