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They are certainly available as an option (along with the reservations IIRC) on webTIS based planners (i.e. the system used by East Coast, Southern, Southeastern, and London Midland).
On East Coast site (& I assume the others as well), Plus Bus is offered as an option during the booking process.
You initially select the rail portion of the journey & later on you can choose to select the plusbus add-ons for your origin & destination rail stations (if appropriate for those stations) on those days of travel for both outward & return portions.
The plus bus portion is then issued on a separate ticket (e.g. Cambridge to Cambridge Plus bus)
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