The growing interest in the use of luminescence thermometry for noncontact temperature reading in very specific conditions imposes the need to develop an approach allowing modification of the luminescence parameters of the thermometer accordingly to the requirements. Therefore, in response to these expectations, this manuscript reports an approach to modulating the spectral position and the luminescence thermal quenching rate of Fe3+ ions by modifying the crystal field strength and the host material composition of nanocrystalline AB2O4 type nanocrystals (A= Mg, Ca; B=Al, Ga). It was proved that in a group of MgAl2O4, MgGa2O4, CaAl2O4, and CaGa2O4 nanocrystals doped with Fe3+ ions the emission spectral range, as well as the relative thermal sensitivity (from 0.2%/oC for MAO to 2.07%/oC for CGO) and the operating temperature range, can be easily modified by the host material composition. For instance, a maximal relative thermal sensitivity of 2.58%/oC is obtained for Fe3+, Tb3+ co-doped CaAl2O4 nanocrystals. The proposed approach is a step toward the intentional designing of the highly sensitive luminescent thermometer.