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This study deals with the fine tuning of the photophysical characteristics, and especially two-photon absorption (2PA) properties, of several homo- and heteroleptic ruthenium(II) complexes involving 5-substituted-1,10-phenanthroline ligands. The 2PA spectra of the complexes were determined in the 700–930 nm range by investigating their two-photon excited luminescence (2PEL). Structure – linear and nonlinear optical properties correlations are discussed, and potential applications (therapy and optical power limiting in the near infrared) can be anticipated.