A couple reasons. First, as good as Gray's defenses were with the Bills in 2003 and 2004, they weren't so hot in 2005.
Second, Gray tried to become a HC, and notably lost to Kubiak here for that opportunity. He then interviewed to be the DC in Green Bay, but that job went to someone else. I think the coaching musical chairs were nearing the end by the time Kubiak was hired in 2006.
Lastly, Gregg Williams in Washington wanted him back. Gray had worked with Williams in Tennessee and again in Buffalo. Plus, I am guessing Dan Snyder probably was willing to pay Gray like a DC to be his DB coach.
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