FOPP in Covent Garden is the go-to - it's an offshoot of HMV but with more back-cat and less merch/ancillary goods. Also has plenty of sales (atm inc. 88 Films, Arrow, Final Cut to name a few).
Foyles up the road from it has a good selection of Eureka titles (which neither HMV nor FOPP stock in-store) and a great film books section.
Further up the road from the aforementioned are two CEX stores, primarily second-hand tech/games and with diminishing BD/DVD sections, but always worth a browse for the occasional bargain or OOP find.
Further out in Southbank is the British Film Institute with its own small store - not very competitive prices, but a nice store nonetheless and obviously has considerably stock of BFI releases.
After that, you also have Notting Hill Music and DVD Exchange - only has a tiny BD section generally but a lot of cheap DVDs and a ton of VHS tapes if you're into that. Also a great soundtrack selection on CD/LP.
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