An absolute thermal lens method to determine fluorescence quantum efficiency and concentration quenching of solids is described in this work. The quantum efficiency of low silica calcium aluminate glasses doped with different concentrations of neodymium dioxide and melted under vacuum conditions to remove water has been measured by using mode-mismatched thermal lens spectrometry. It has been shown that the thermal lens signal amplitude is linearly dependent on neodymium concentrations up to 4.0 wt %, changing significantly from 4.5 to 5.0 wt %, indicating that there was quenching of the fluorescence only above 4.0 wt % neodymium dioxide. The quantitative treatment for the thermal lens effect provided the absolute value of the sample’s fluorescence quantum efficiency. The technique is simple to perform and can be applied for a wide range of fluorescent materials.