Polyoxometalates (POMs) have fascinating structures and promising properties. The arsenomolybdates, as an important branch of POMs, are outstanding photocatalysts for organic dyes. In this work, we selected organic dyes to evaluate the photocatalytic activity of arsenomolybdates under UV light, containing compared with photocatalytic activity of different structural arsenomolybdates, stability, and the photocatalytic reaction mechanism of arsenomolybdates as photocatalyst. The arsenomolybdates may be used to as environmental photocatalysts for the degrading of organic dyes and solving the problem of environmental pollution.