I’m sure
@RELL6L might have a few ideas
Well, first of all I have to confess I have not explored South West Scotland for many years and not at all by bus, apart from one trip Kilmarnock to Dumfries as part of a circuit from Glasgow. But I have done some research on the area in case the opportunity ever presents itself, which I still hope it might. Opinions are my own….
Obviously in part this depends on what you like, coastal scenery, inland scenery, attractive towns and villages etc. Starting with the coast, the 58/60/358/360 services from Ayr to Girvan and Stranraer are good. Ayr is an attractive large town, Girvan an attractive small town and definitely worth breaking a journey here. The 60/360 via Turnberry is probably slightly preferable to the 58/358.
From Stranraer the Rhins of Galloway peninsula to the west is difficult to explore by bus with infrequent services but a trip on the 367 over to Portpatrick and back might be possible. Carrying on round the coast the Stagecoach 416/415 from Stranraer to Port William and then on via the Isle of Whithorn and Wigtown to Newton Stewart is excellent scenery. If you can time it right it is possible to break your journey a few times on this section, most importantly at Wigtown. I think the 500 trunk service across from Stranraer to Dumfries has good scenery but it is a main road and not as spectacular. You really have no choice but to use the 500 to go east of Newton Stewart but then you can take coastal options via Kirkcudbright, a lovely town, and on from there via Dalbeattie and Sandyhills to Dumfries. Good, but not as good as the coast west of Newton Stewart.
Heading inland the great routes include the ones you have identified. The 520 between Castle Douglas and Dalmellington, only twice a day, is great and was reviewed in post 880 of the trip reports thread not long ago. You then head north to Ayr on the 52 or east to Cumnock on the 356. The 359 runs sort of parallel further west between Newton Stewart and Girvan and also is well worth riding to complete a circular trip via Stranraer.
The route across from Ayr to Cumnock is former mining territory and, frankly, less attractive, both in terms of scenery and places. However, one you have already spotted, is going to Wanlockhead. The Brownrigg 221 will take you from Sanquhar to Wanlockhead and then the 30/31 from there to Lanark. Connections aren’t brilliant but if you leave Cumnock for Sanquhar on the 246 at 07.45 on a schoolday, this is normally a double deck coach, then take the 221 to Wanlockhead and the Stuarts 31 to Lanark and you are there at 11.00 with a little time for each change. Return probably via Glasgow. On a good day this is definitely spectacular.
Hope this helps!