The first time she toured through Portland, Lizzy Plapinger saw a “Japanese work-of-art jacket” at a local vintage shop — but passed it up.

The lead vocalist for MS MR, a duo known for its lovely secondhand threads, went back on tour, but Plapinger couldn’t forget about the coat.

“I talked about it for essentially a year and a half,” she said, laughing. “And then the next time I came around to Portland, they still had it and I bought it! I still have that jacket.”

When she and Max Hershenow play the Crystal Ballroom Oct. 21, they’ll bring a sound as unique as their fashion sense. Plapinger’s gorgeous, husky vocals and Hershenow’s nuanced electronic canvases feature colors as exotic as the furs, leather clothes, and Technicolor hair featured in the band’s promotional photos.

MS MR’s lyrics and the emotional pacing of their songs can take the music to macabre places — so it’s fitting a track from their new album “How Does It Feel” is featured on the spine-tingling trailer for this fall’s feature film “Room,” based on the best-selling novel by Emma Donoghue.

“I think the balance between light and dark in the music and the lyrics and the message has always been the greatest balancing act of the band, artistically,” Plapinger said. “The first record was super candy colored, but it had such sort of gothic and macabre and dark undertones. And I think still on (‘How Does It Feel’) even though we’re maybe more in like a jewel-tone, saturated landscape, sometimes the most positive songs are hidden within a dark and brooding atmosphere and vice versa.”

The Columbia recording artists and Vassar College alums started out cultivating mystery with anonymous releases on tumblr before their 2013 debut, “Secondhand Rapture,” which peaked at 116 on the Billboard 200 chart. Plapinger also launched a successful boutique record label, Neon Gold, home to artists including Tove Lo and Charli XCX.

Hershenow and Plapinger are honest about their high ambitions — headlining the UK’s Glastonbury music festival, for example — but also in danger of a sophomore slump. The new album hasn’t quite lived up to high expectations, and Pitchfork called it “timid.”

“I don’t think it’s fair to put us next to Top 40 music when truly I think a lot of the time we are saying things that are more intellectual or layered than just going to the club and popping bottles,” Plapinger said.

Yet MS MR’s new material is more pop-oriented, more complete and detailed. The tunes grow on you, but they’re not as raw or as bold as the band’s early material. The best number, “Painted,” channels synth washes and pulsing basslines into a syncopated Latin piano hook. The repeated lyric “What did you think would happen? / When you put me in unnatural space?” could be a reference to the duo’s recording process.

Hershenow said the pair first tried writing in top-notch studios, but ended up retreating to humbler digs.

“We actually function best in a place that’s totally DIY where we retain absolute control,” he said. “We wrote it in a … little hole in the wall.”

Perhaps MS MR’s “do it yourself” preference and need for down-to-earth surroundings parallels the duo’s taste for vintage clothing. If so, Portland certainly won’t disappoint.