This study investigates the effects of thermal aging on the crystallographic texture, dislocation density, and tensile behavior of a novel high entropy alloy (HEA) with the composition Al2Fe53Ni35Cu5Ti5 (at.%). Using a combination of X-ray diffraction (XRD) and high-resolution electron backscatter diffraction (HR-EBSD), three different heat-treated configurations (ConFig 1: water-quenched; ConFig 2: aged 3 h at 530 °C; ConFig 3: aged 10 h at 530 °C) were characterized to correlate microstructural evolution with mechanical performance. The alloy displayed a primarily FCC structure across all treatments, with progressive formation of Ni₃Ti (HCP) and AlNi₃ (L12) precipitates during aging. Lattice distortion, initially severe in the as-cast state, reduced significantly with aging, as reflected in the transition toward near-cubic symmetry. Dislocation density followed a nonlinear trend, decreasing in ConFig. 2 due to recovery but rising in ConFig. 3 with the formation of a secondary phase. Texture analysis revealed a dominant {001} < 100 > component in early stages, shifting toward a pronounced Goss ({110} < 001 >) orientation with prolonged aging. Correspondingly, tensile testing showed an increasing yield and ultimate tensile strength from 250/334 MPa in ConFig 1 to 400 MPa/465 MPa in ConFig 3, accompanied by a drop in elongation from 55% to 28%. These findings highlight the critical role of precipitation and texture evolution in tuning the strength–ductility balance of HEAs through controlled thermal processing.