Although Atlanta-bred, Miami- and New York City-based singer Chan Marshall (aka Cat Power) has been high on the critical radar since the mid-’90s, much of the attention has focused on her fragile demeanor — live shows have often seen her in near-­catatonic states, paralyzed by stage fright — than on the four exquisite albums she’s released for the Matador label. Her latest, the cheekily titled The Greatest, has been tipped as an attempt at some sort of commercial breakout — logical, considering it follows 2003’s You Are Free, a wide-ranging set of songs that hinted at a restless creative spirit and the work of one not inclined to forever remain consigned to the indie-rock ghetto. This time out, Marshall enlisted Grammy-winning producer Stuart Sikes (White Stripes, Loretta Lynn) and traveled to Memphis to record with an array of noted soul sessioneers, including Al Green sidemen Teenie and Flick Hodges.

While that setup would have most thinking she intended the album as her version of Dusty in Memphis, the record really isn’t that removed from her previous work. Granted, the greasy sonic aphorisms and “shoo-ba-doo” backing that color “Lived in Bars” are a nod to her Southern surroundings, as are the parping brass hooks that highlight “Could We” (though the latter track is ultimately more Irish R&B, à la Van Morrison, than Memphis soul stew). As with Free, she takes things in manifold musical directions here, twanging her way through the keening country-fiddle tune “Empty Shell,” pertly navigating the reggae-jazz rhythms of “Willie,” cribbing Henry Mancini’s “Moon River” melody for the title track, and saving her tenderest mercies for the tear-jerking piano ballad “Where Is My Love?” While much of the album is steeped, if not dripping, in a kind of languid blues, thankfully, Marshall doesn’t strain to adopt some faux vocal persona, keeping her signature gauzy phrasing and delivery intact. A near-perfect marriage of mood and music, the record may not catapult Marshall to the top of the pop heap, but it’s certain to win her a few new fans.