Luminescence thermometry is a remote temperature measurement technique that relies on thermally induced changes in spectroscopic properties. Because of its great application potential, even under very demanding conditions where other techniques fail, it has attracted the attention of many researchers in recent years. Unfortunately, most of the existing luminescence thermometers are fraught with large inaccuracies and thus are not reliable enough to be applied in real and demanding applications. However, there is one of the most recent and very promising but insufficiently studied approaches to luminescence thermometry quantification – single-band ratiometric luminescence thermometry. It is based on the analysis of the luminescence intensity ratio of a single emission band being photoexcited in two ways, i.e. by ground (GSA) and excited (ESA) state absorption. It is characterized by high relative sensitivity to temperature changes as well as high measurement precision. However, because ESA-excited luminescence intensity can depend on the type and concentration of dopant ions or the properties of the host material, further more-detailed studies must be conducted to understand the impact of numerous photophysical processes on the relative sensitivity, temperature resolution and useful temperature range of SBR LTs. In this work, the effect of interionic interactions occurring through cross-relaxation on the thermometric properties of single-band ratiometric luminescent thermometers in NaYF₄:Nd³⁺ and NaGdF₄:Nd³⁺ was investigated and discussed. In contrast to the disadvantageous concentration quenching phenomenon that is typically observed at an increased content of dopants, the beneficial role of cross-relaxation in the enhancement of the signal-to-noise ratio of the ESA-excited luminescence at high temperatures was demonstrated. The maximum relative temperature sensitivity reached was equal to S_R = 16.9% K⁻¹ at 223 K for NaYF₄:50%Nd³⁺ nanocrystals and its value remained above 1% K⁻¹ throughout the whole analyzed temperature range from 223 K to 473 K.