No, memory is only useful in the contexts of the processor which uses it, remember that all high speed memory is connected to some kind of processor, with system RAM it's connected directly to your CPU, so the CPU reads out of this RAM, calculates values and puts the results back into RAM.
Same for the GPU, the GPU reads directly from vRAM and does calculations and stuffs the results of those back into vRAM.
The link (Bus) between the CPU and RAM, or the GPU and vRAM is extremely high speed in order provide such fast processors with a constant flow of data, the link between the GPU and the rest of the system such as the CPU, runs over a relatively slow and laggy bus (the PCI-E bus)
The only real way you can make use of vRAM is when you actually do the calculations on the GPU itself, which we're doing more and more, you'll see hardware accelerated video playback, hardware accelerated flash player in browsers, and other such things, there's also lots of other specialized apps which can use the GPU and in fact run much faster on a GPU like bitcoin mining, password cracking and things like that.
Generally speaking the GPU is much better at specific tasks, those which are highly parallelizable and so it's these kinds of tasks that people tend to build GPU apps for. Outside of that, there's no easy way to use vRAM as extended system RAM, it's just too far away from the CPU, to slow and too laggy to be of any use for real time processing, there's already solutions for extending system RAM and that's using a pagefile on the HDD or SSD.