Crosscountry, would like to see Peterborough to Stansted Airport Stansted Express also (from Stansted Airport to Liverpool Street and Stratford station with the British Rail Class 745 FLIRT
EMR Corby to St Pancras, could be set pre or post electrification so you could have 360s or HSTs and 222s on it, and if Thameslink's licence ever came about the 700s or 319s from Bedford
Out of those operators I voted Transpennine. Nowadays they have a fantastic mix of rolling stock and services. You could have: High speed expresses with the Class 802 on the ECML from York to Newcastle. Or alternatively high speed runs on the Northern section of the WCML in the brand new Class 397s. Relaxing loco hauled runs through the countryside on the Class 68 from York to Scarborough. Semi fast regional services in the 185 between Manchester and Leeds (I'm aware this route is already in the game, but it's just an example), as well as commuter services between busy cities like Liverpool and Manchester. There's a lot of variety, and I'd love to see the operator represented in the game.