This is something that came about from my watching both the original Saturday morning run of episodes and Friday Night Videos back in the 1980s, attaching various pop radio songs to certain episodes. So far I can think of these candidates:Styx's "Mr. Roboto" -- "The Clockwork Smurf"
Peter Schilling's "Major Tom" -- "The Astrosmurf"
Nena's "99 Red Balloons" -- "The Purple Smurfs" (maybe a parody version: "99 purple Smurfs hopping up and down my turf,...")
Sheena Easton's "Telefone" -- "The First Telesmurf"
Weird Al's "Eat It" -- "Greedy And The Porridge Pot"
Cyndi Lauper's "True Colors" -- "The Color Smurfy"
Madonna's "Who's That Girl" -- "The Smurfette" and "Smurfette Unmade"
The Waitresses' "I Know What Boys Like" -- "Romeo And Smurfette"
Weird Al's "Fat" -- "Gourmandizing Greedy" and any episode Bigmouth appears in
Weird Al's "You Think I'm A Clone Now" (a parody of Tiffany's "I Think We're Alone Now") -- "Smurfiplication"
Electric Light Orchestra's "Turn To Stone" -- "Petrified Smurfs"
Sammy Hagar's "I Can't Drive 55" -- "The Smurfbox Derby"
"Hair" from the musical Hair -- "Smurfette's Golden Tresses" and "Symbols Of Wisdom"
The Guess Who's "No Time Left" -- "No Time For Smurfs"
Phil Collins' "Against All Odds" -- "Handy's Sweetheart" (appropriate for a mismatched love relationship!)
Cyndi Lauper's "Change Of Heart" -- "Hefty's Heart"
Eurhythmics' "Sisters Are Doing It For Themselves" -- "Sister Smurf"
Kiss' "I (Believe In Me)" (from Music From The Elder) -- "A Little Smurf Confidence"
Hanson's "Mmmbop" -- "The Smurflings" (okay, this is a decade out of time, but don't the Hanson boys sound like Smurflings?)
Any songs you can think of that would be appropriate for certain episodes?