Ru(ii)-based photoactivated chemotherapy (PACT) agents are promising; however, their short wavelength absorption (generally <550 nm) and poor tumor accumulation ability limit their in vivo applications. Herein, bovine serum albumin (BSA) coated lanthanide-doped upconversion nanoparticles (NaYF4:Yb:Tm@NaYF4 (UCNPs)) were loaded with a Ru(ii) PACT agent, i.e. [Ru(dip)2(spc)]+ (dip = 4,7-diphenyl-1,10-phenanthroline; spc = 2-sulfonic acid pyridine-3-carboxylic acid). The resultant UCNP@BSA@Ru can transfer [Ru(dip)2(spc)]+ to tumor cells in vitro as well as tumor tissues in vivo highly efficiently and selectively owing to the targeting ability of BSA and the enhanced permeability and retention effect of the nanoparticles. The subsequent near infrared (NIR) light irradiation at 980 nm or visible light irradiation at 470 nm can initiate dissociation of the spc ligand, and the released Ru(ii) aqua compounds ([Ru(dip)2(H2O)2]2+) may exert a potent cytotoxicity towards a series of cancer cells but a much weaker effect on the normal IOSE80 cells. The in vivo (mouse) results showed that UCNP@BSA@Ru could inhibit tumor growth upon 980 nm irradiation more efficiently than in the dark and more efficiently than cisplatin (in the dark).