Nd,Cr:Gd3Sc2Ga3O12 (GSGG) thin films have been produced for the first time. They were grown on Si(001) substrates at 650 °C by pulsed laser ablation at 248 nm of a crystalline Nd,Cr:GSGG target rod. The laser plume was analyzed using time-of-flight quadrupole mass spectroscopy, and consisted of elemental and metal oxide fragments with kinetic energies typically in the range 10 to 40 eV, though extending up to 100 eV. Although films deposited in vacuum using laser fluences of 0.8+/-0.1 Jcm-2 reproduced the Nd,Cr:GSGG bulk stoichiometry, those deposited using fluences above 3 Jcm-2 resulted in noncongruent material transfer and were deficient in Ga and Cr. Attempts to grow films using synchronized oxygen or oxygen/argon pulses yielded mixed oxide phases. Under optimal growth conditions, the films were heteroepitaxial, with GSGG(001)∥Si(001), and exhibited Volmer-Weber-type growth. Room-temperature emission spectra of the films suggest efficient non-radiative energy transfer between Cr3+ and Nd3+ ions, similar to that of the bulk crystal.