The original UNDER NIGHT IN-BIRTH Exe:Late soundtrack by Raito is where all those killer character themes first dropped and honestly they came out swinging from day one. This is the PS3 and arcade version before the [st] update, and it opens with "starry night prison" which has this moody, atmospheric intro that sets the whole tone.
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"Night Walker" for Linne is tight and aggressive with these rapid guitar riffs. "Purity & Strictly" gives Orie this elegant but intense energy, mixing clean melodies with driving beats. "Overwhelm Despair" for Hilda goes full dramatic villain.
The core roster themes here are the foundation everything else built on. If you're getting into UNI for the first time, this is ground zero for understanding why the music hits so hard.