I was visiting Harvard as a prefrosh when I first heard Belle and Sebastian. After my long first night on campus, I woke to the opening strains of their breakout album “If You’re Feeling Sinister,” coming from my host’s CD-player alarm clock. As rain ran down the windows of the Lionel common room, I fell in love.

It turns out I wasn’t alone. “If You’re Feeling Sinister” and several subsequent albums won the Scottish septet a legion of fans with catchy, precocious songs narrating the lives of misfits. This is, however, no dour affair, as frontman Stuart Murdoch’s lyrics seek joy in life’s absurdities and love’s awkwardness. The songs run the gamut from the light and poppy to the sweetly sad, consistently delivering pitch-perfect charm.

While the band’s last release, 2003s “Dear Catastrophe Waitress,” stressed the former with instantly-catchy songs and goofy lyrics, their new LP, “The Life Pursuit,” has more gravity to match its sober title. Through the first four listens, I was disappointed with the album; by the seventh, I had fallen in love with the band again.

Part of that reaction has to do with the fact that “The Life Pursuit,” unlike previous work, was recorded in more or less live sessions rather than as layers of separately recorded instrumental tracks. The harmonies are less layered, the arrangements simpler. Instead, the album relies more on improvisation and musical solos.

The press materials say this is a more “muscular” approach—but that’s not quite right. It’s lithe and subtle and exuberant. Despite the lackadaisical image the band likes to project, they are seven seriously talented musicians. It’s gratifying, then, that they’ve found success in a production strategy that lets them react to each other in the studio. That sense of playful collaboration rewards more and more with each listen.

Lyrically, Murdoch sticks to what has worked in the past: stories about misfits. The title character of the song “Sukie in the Graveyard” spends her time making grave rubbings, lives illegally in the attic of an art school she’s not enrolled in, and poses for life-drawing classes with “the grace of an eel, sleek and stark.” And when the narrator of “Funny Little Frog” sings to his love that “you’re my picture on the wall/you’re my vision in the hall,” he’s not using a metaphor; the poor bloke’s having a relationship with an imaginary friend.

While it often grasps at the sublime, “The Life Pursuit” falls short of greatness. It could have been a perfectly crafted EP—of which this band has already made several—had the disc’s filler been culled.

While on balance the good outweighs the bad, it remains hard to sit through the clunkers, such as “To Be Myself Completely,” whose vague lyrics and generic melody drag down the last third of the album. This is most likely because it’s the album’s one song on which guitarist Stevie Jackson replaces Murdoch on lead vocals. Unfortunately, Jackson just isn’t a lead singer; where Murdoch is silky-smooth, Jackson’s singing sounds distractingly strained.

“The Life Pursuit” probably isn’t the big-time hit that Belle and Sebastian deserve, as their new, more mature sound takes them another step away from the mainstream.

Still, the new LP has plenty of hummability. If you’re a fan of the band, you should buy this album for “Sukie” alone; it’s a fun, sassy, organ-driven romp that’s destined to become a staple of their live shows. And if you haven’t yet discovered Belle and Sebastian, do yourself a favor and pick up “If You’re Feeling Sinister.” Your rainy days will improve tremendously.­

—Staff writer Michael A. Mohammed can be reached at mohammed@fas.harvard.edu.