This dataset contains hyperspectral imaging (HSI) and fluorescence lifetime imaging microscopy (FLIM) acquisitions of NIH-3T3 fibroblast cells stained with the membrane probe LAURDAN (6-dodecanoyl-2-dimethylaminonaphthalene). The data were generated and analyzed in the study “A multidimensional phasor approach reveals LAURDAN photophysics in NIH-3T3 cell membranes” (DOI: 10.1038/s41598-017-08564-z). These measurements were used to demonstrate multidimensional phasor analysis, a model-free approach that combines spectral and lifetime information at the pixel level. This methodology enabled the separation of polarity effects from dipolar relaxation in cellular membranes and revealed the heterogeneous photophysics of LAURDAN across different membrane regions. The dataset can be used to reproduce the analyses presented in the publication and as a reference resource for developing or benchmarking spectral, lifetime, and multidimensional phasor analysis methods in bioimaging. For the FBD files, a laser frequency factor of 0.99168 is recommended to ensure correct reading.