A positive electrode active material for a non-aqueous electrolyte secondary battery, according to an example of this embodiment, includes a lithium transition metal composite oxide which has a layered structure and contains at least Ni, Al, and Ca. The lithium transition metal composite oxide has a Ni content of 85-95 mol %, an Al content of at most 8 mol %, and a Ca content of at most 2 mol % with respect to the total amount of metal elements other than Li. In addition, the proportion of metal elements other than Li present in a Li layer is 0.6-2.0 mol % with respect to the total amount of metal elements other than Li contained in the composite oxide.