The Decemberists’ frontman Colin Meloy has an English degree with an emphasis in creative writing, perfectly apt for a songwriter with awe-inspiring vocabulary and majestic imagery, not to mention original style. The band’s peculiar brand of folk-inspired pop is known for Meloy’s mellifluous, theatrical storytelling (on “Picaresque,” their third album, he explores a murder-suicide in the belly of a whale, along with Victorian orphans, as always). The new album, sprinkled with gems, is an adept example of the Decemberists’ heralded ability to craft glorious pop music, a wonderful paradigm of compelling erudition that demands obsessively repeated listens.

Though only recently generating mainstream media buzz as a “hot new band,” the Decemberists have been turning hip heads since the release of their dynamically stirring 2002 debut, “Castaways and Cutouts.” Like the similar cult favorite Neutral Milk Hotel, the band has consistently utilized unique instrumentation — from eerie accordions to twangy pedal steel guitars, dulcimers and the theremin. After the intimate and cerebral “Her Majesty,” the band released “The Tain EP” in 2004, a Bob Dylan and even Black Sabbath-infused 18-minute epic based on an eighth-century Irish poem.

“Picaresque” is no less of a concentrated effort in musical and literate dexterity, and it is a superb success at that. “Eli, the Barrow Boy,” a solemn folk song about children and ghosts, perfectly conveys the deep sadness and tediousness of a daily routine after a great loss. The wistful wailing of the chorus, accompanied by drummer Rachel Blumberg’s elevated harmony, is as moving as anything the band has done: “Would I could afford to buy my love a fine robe … But she is dead and gone and lying in a pine grove / And I must push my barrow all the day.”

“On the Bus Mall,” is another ode to the loss of innocence. The song starts off with Meloy strumming an steel-stringed guitar, over which multi-instrumentalist Chris Funk (his Christian name) gorgeously picks an electric guitar. Drums and organs come in as the song builds over six lovely minutes, evoking a tone that’s perfect for the gray and cold week following a day on which everyone thought spring had sprung.

As good as the Decemberists are at soothing and reflective tracks, their upbeat songs — like their most popular, “July, July!,” from “Castaways” — showcase the band’s excellent pop sensibilities. “The Sporting Life,” which sounds like Belle and Sebastian at their best, is fueled by a big band bouncy rhythm (though, of course, it’s about humiliation and disappointment). “Sixteen Military Wives” is a rollicking condemnation of war hawks, fueled by a fun-poking chorus of roaring baritone saxophones, bright trumpets and pounding electric pianos. The song features a music video, part-United Nations and part-Wes Anderson, that might even be sweeter than the song itself.

Another highlight is “The Mariner’s Revenge Song,” a testament to the band’s epic storytelling, which weaves anecdotes of the absurd with a nefariously edged accordion. The track sounds more like a song from a musical, complete with echoing effects and background tambourines synched up to the crux of the storytelling. Then there’s “(From My Own True Love) Lost at Sea,” a warm, druggy ballad that pulses with a quiet gong-like beating.

A large part of the Decemberists’ charm comes from fantastically strange pop songs with fantastically exotic instrumentation. “Picturesque,” thankfully, is the most fully orchestrated album of the three LPs. “We Both Go Down Together” (whose opening sounds suspiciously like REM’s “Losing My Religion”) features a splendid orchestra in the background and an impeccable violin. But that’s nothing compared to the unmatched prettiness of the sing-along chorus.

The near-perfect album is slightly tarnished by “The Infanta,” a forced song with too much going on to be likeable. Led by an urgently jittery beat, this track is annoyingly thunderous, missing the suspenseful drama that it goes for. But if “Infanta” is a disappointing opener, “Of Angels and Angles” is the perfect closer. Hushed by an acoustic guitar’s sweet arpeggios, the brief song ends the album on a note of tragedy: “As on we go drowning, / Down we go away.”

Albums that are this obviously ambitious usually end with disappointment. But “Picaresque” does otherwise, proving to be endlessly original, expectedly inventive and remarkably accomplished. The Decemberists’ sophistication makes for polished and precise music, but the album is poignant and full of passion. The young band’s characteristic creativity has made a deeply resounding and happily untiring album, yet again.