When in Penzance, I would suggest that you take the short train ride to St.Ives. To do that, you need to change at St.Erth from the mainline to the St.Ives branch line. Buy on the day a return ticket for about £5.
https://www.visitcornwall.com
http://www.railrover.org/pages/cornwall-ranger.html
When in Falmouth, try & list Trebah Garden and maybe Glendurgan. https://www.trebahgarden.co.uk
https://www.nationaltrust.org.uk/visit/cornwall/glendurgan-garden
If you are into trains, you might like to take a ride on >https://www.southdevonrailway.co.uk
To do this, you would travel to Totnes (on the mainline) to transfer to the heritage steam railway. Totnes is also an attractive town to look around or stay a night or 2. Ferries also go from Totnes down the estuary to Dartmouth. In fact, you can buy a special ticket that includes the ferry plus another steam train from Dartmouth / Kingswear to Paignton and your journey back to Totnes. (Your trains to/from Cornwall will stop at Totnes).
2 railways go from Exeter to London with the fastest being the GWR to Paddington. The other one is South Western Railway which goes to London Waterloo. This route uses diesel multiple units with underfloor engines.
It is perfectly viable to travel back from the south west via Bristol (Temple Meads is the main station). But, I would suggest you go to Bristol and change for the short hop to Bath and stay a night or 2 before heading back to London. That will give you a different line between Taunton & Reading compared to the one you travelled out on.
Video - London to Bath by Train.https://www.youtube.com/watch?v=xpp6vAs2W4I
You may like to get a 2 *Together Railcard for £30 as this will reduce fares by a third. You will find the cheapest prices for the longer journeys by pre-booking Advance tickets (not refundable) for specific trains around 11 weeks out. Also note that it is sometimes cheaper to split the ticket. These 2 sites will tell you if splitting is cheaper. On trainsplit - click ‘Proceed’ and it will tell you the splits and prices for each leg. As a guide, you should be able to get from Penzance to Bath for £32.61 departing at 9.25 (non Railcard price) tested today for Tues 7 February. * Not valid weekdays before 9.30am.
https://v3.trainsplit.com
https://www.traintickets.com/?/