In terms of the bus width / speed of the memory, the only thing that matters is memory bandwidth. This is easy to calculate.
HD 4870 = 3600MHz GDDR5 * (256-bit/8000) = 115.2 GB/s
GTX 260 = 2000MHz GDDR3 * (448-bit/8000) = 112.0 GB/s
The HD 4870 has slightly more memory bandwidth than the GTX 260, but the two get their high memory bandwidth in different ways. The GTX 260 relies on a very wide bus but slow memory, meanwhile the HD 4870 relies on very fast memory connected to the GPU via a fairly narrow bus. Airhendrix13's explanation of this can help you visualize the difference.
As for the amount of VRAM, 512MB vs 896MB, they cannot be directly compared in this case. For nVidia GeForce cards, >512MB of memory seems to make a difference in certain situations. Theoretically more memory should give you better performance in high-res / AA+AF situations, but the GTX 260 doesn't seem to have any advantage in these scenarios over the HD 4870. AMD's cards use VRAM much more effectively, so they can do just as well with 512MB of memory as nVidia's cards can do with 896MB.
These benches can help show what I am talking about:
http://www.pcgameshardware.de/...enchmark-Test/&page=10
Oblivion at high-res + Quarl's texture pack certainly consumes a lot of VRAM, yet the HD 4870 dominates here at high res + AA/AF.