Fe2SiS4 and Fe2GeS4 crystalline materials posses direct bandgaps of ∼1.55 and ∼1.4 eV respectively and an absorption coefficient larger than 105 cm–1; their theoretical potential as solar photovoltaic absorbers has been demonstrated. However, no solar devices that employ either Fe2SiS4 or Fe2GeS4 have been reported to date. In the presented work, nanoprecursors to Fe2SiS4 and Fe2GeS4 have been fabricated and employed to build ultra-thin-film layers via spray coating and rod coating methods. Temperature-dependent X-Ray diffraction analyses of nanoprecursors coatings show an unprecedented low temperature for forming crystalline Fe2SiS4 and Fe2GeS4. Fabricating of ultra-thin-film photovoltaic devices utilizing Fe2SiS4 and Fe2GeS4 as solar absorber material is presented.