In this paper, we successfully synthesized 3D graphene aerogels-supported Ag and Ag@Ag3PO4 heterostructure (3D Ag/Ag@Ag3PO4/GA) by the hetero-growth of Ag3PO4 on partly Ag nanoparticles in macroporous 3D graphene aerogels (3D GA), aiming for the efficient adsorption-photocatalysis capture of both cationic (RhB, MB, and NR) and anionic (MO) dyes from aqueous solutions. For the removal of different dyes, the contributions of adsorption and photocatalysis is different and the apparent removal sequence is NR > RhB > MB > MO on the prepared 3D Ag/Ag@Ag3PO4/GA. Compared with bare Ag3PO4 particles, Ag3PO4/GO, and Ag/Ag@Ag3PO4/ GO, the prepared 3D Ag/Ag@Ag3PO4/GA exhibits the highest catalytic activities for the visible light degradation of RhB and MO. The possible mechanism for improved photocatalytic degradation of dyes by the 3D Ag/Ag@Ag3PO4/GA is proposed based on the active species trapping experiments. Moreover, the good stability and convenient recycling of the prepared 3D Ag/Ag@Ag3PO4/GA composite further make it have potential application prospect in eliminating organic contaminants.