A valerolactone compound represented by the formula (I): ##STR00001## wherein each of R.sup.1 and R.sup.2 is independently a hydrogen atom, a methyl group or an ethyl group wherein when R.sup.1 is a hydrogen atom, R.sup.2 is not a hydrogen atom; and wherein when R.sup.2 is a hydrogen atom, R.sup.1 is not a hydrogen atom, R.sup.3 is a hydrogen atom or a methyl group, and R.sup.4 is a propyl group, a 1-propenyl group or a phenyl group; a valerolactone compound represented by the formula (II): ##STR00002## a process for preparing the same; and a perfume composition comprising the above-mentioned valerolactone compound.