The authors agree that this surname derives from Greek, with the sense of "beautiful" or "good". E. Rossoni considers it probably a graphic variant of Calì (without accent), derived from the Greek word kalos ("beautiful") and from its abbreviated form kalìs, and places it especially in the Catania and Palermo areas, in Sicily.

G. Rohlfs specifies the etymon as the Greek καλή ("the good one"), of Greek-Byzantine origin, noting that the form Καλῆς still survives as a surname in Greece. Rohlfs documents the surname in Calabria: in the province of Cosenza (Fuscaldo), the province of Catanzaro (Guardavalle and Vibo) and the province of Reggio Calabria (Caulonia, Laureana).

V. Blunda adds that the Greek term calì is the feminine form of calòs, parallel to the surname Calá, and that in Sicily it functioned originally as a nickname referring to a female ancestor for her beauty or goodness, before becoming a family surname. G. P. Holmes agrees on the positive sense of the term, which he describes as an "auspicious name" of medieval Greek origin.