Raw data for the manuscript 'Orbital-Selective Hybridization Shapes the Electronic Structure of Layered Antiferromagnetic CrPS4' The AFM and Raman data are provided as .txt files. The ARPES data are provided as .itx files, which can be analyzed using Igor Pro or Python ARPES packages. The data is sorted by sample and temperature. Sample 1 was investigated using a monochromatized helium lamp at 21.2 eV, while sample 2 was investigated using a pulsed high-harmonic generation source at 26.4 eV. For further requests or elaboration on the data analysis, please contact the corresponding authors. Appearance Index: 'AFM' -> SI Fig. S1 'Raman' 'Irradiation_Study' -> SI Fig. S2.1 'Polarization_Study' -> SI Fig. S2.2 'Raman_ARPES_spot' -> SI Fig. S1 'Photoemission_Sample_1' '10K_ARPES_valence_band' -> SI Fig. S6.1 '300K_ARPES_valence_band' -> Fig. 2, 3; SI Fig. S5, S6.1, S6.2, S7.1, S7.2 'CrPS4_sample1_PEEM' -> Fig. 2 'CrPS4_sample1_WKF' -> SI Fig. S3 'Photoemission_Sample_2' '7K_ARPES' -> SI Fig. S6.1 'CrPS4_sample2_7K_ARPES_valence_band_and_EDC' -> Fig. 4; SI Fig. S6.1, S6.2 '300K_ARPES' 'CrPS4_sample2_300K_ARPES_valence_band' -> Fig. 4; SI Fig. S5, S6.2 'CrPS4_sample2_300K_EDC' -> SI Fig. S6.1 'CrPS4_sample2_PEEM' -> Fig. 4