" And am hoping that upgrading to the F36 is the smarter choice than adding a sub that would seamlessly integrate. Any thought would be appreciated. Thank you."
I wouldn't trade the 1's for a pair of F36's. I've heard them side by side and the Vandersteen is a better speaker. If you get a Vandersteen sub, you can plan on keeping it for a very long time. Its an extremely well thought out design and will work with just about any speaker.
" I have a VPI Scout with Sound Smith Zephyr III Cartridge running into a Musical Fidelity v-LPS that runs into a NAD VISO 5 Receiver and back out to a pair of Vandersteen 1ce's. Since I recently bought the Zephyr III, it revealed some inadequacies, and I am in upgrade mode."
I don't know how many hours are on your new cart, but it will need to be broken in. The difference from new will be significant. However, looking at your system, your NAD is clearly the weak link. You're not hearing what the Model 1's are fully capable of. Its really not the speaker's fault that your system has a lack of dynamics and bass. If you put a better sounding, more powerful amp on the 1's, the change will be huge. The sub is a good idea, but you won't be so compelled to get one with a better amp in place.