Replying back because I shelved this for a bit, then got some test prep and took my exams. Passed both easily.
For prep materials I purchased a book, CompTIA A+ 220-801 and 220-802 Authorized Cert Guide, Deluxe Edition (Soper, Prowse, and Mueller)
http://www.amazon.com/CompTIA-220-801-220-802-Authorize... which paid itself back partway due to the coupon included. The book is of decent length and depth and in color, I thought it was a pretty good resource. A few practice tests were included and those helped put my mind at ease / inform me which areas I was not maintaining.
For the 220-802, I purchased a 30-day use of the MeasureUp practice test. This was not inexpensive, but I thought these topics would be my weaker ones so I wanted a more thorough review. I can definitely say that multiple tries at their testing bank helped, the simulations were good too. On the downside, there were a number of topics on the 220-802 that were not covered in the practice test, so it's a good thing I hadn't used it as my only prep. Also, their software is rather outdated; I was able to run it in Chrome with a "not optimized, you may have issues" warning and was not able to run it in IE at all. How strange for a tech-forward company!
As indicated in my original post, I did a watchthrough of most of the videos on Professor Messer, to which I am thankful. Just watching some videos was definitely not enough to memorize all the command line tools, windows xp paths, networking ports, data transfer rates etc that you are expected to know, though!
Hope this can help a little bit if others find themselves in the same position. Now to figure out how to get all these years of experience in VMWare and IIS setting up Cisco systems that employers seem to want around here. Persevere!