I've found out that some games have limited FPS like Vindictus (60 fps) and Medal of Honor (62 fps) . I've tried turning off vsync and the frame cap is still there. Is there any way to unlock the frame cap using some type of software or tweaking around some type of file?
There is little reason to do this, at least not to achieve a multiple of 60/75/85.
The frame rate you see is often tied to your monitors internal refresh rate, in other words your monitor can probably only output 60 frames per second. Outputting beyond this in non multiples can result in tearing of frames, where it renders two halves of two different frames because they don't line up in refresh rates.
Vertical sync is useful in that it provides a smoother visual for the game.
It should only be turned off if things like input are tied to the frame rate and turning it off would result it more responsive gameplay or you can achieve a higher multiple of your screens refresh rate.
Turning it off won't increase the amount of frames your monitor shows as it has a limit. These limits for LCDs are often 59/60, 75 or 85. CRTs have much higher limits, 120, 200+.