The structure of self-reinforced composites (SRCs) based on ultra-high molecular weight 21 polyethylene (UHMWPE) was studied by means of Wide-Angle X-Ray Scattering (WAXS), X-Ray 22 tomography, Raman spectroscopy, Scanning Electron Microscopy (SEM) and in situ tensile testing 23 in combination with advanced processing tools like Avizo, ImageJ, and Ncorr to determine the cor-24 relation between the processing conditions, on the one hand, and the molecular structure and 25 mechanical properties, on the other. SRCs were fabricated by hot compaction of UHMWPE fibers at 26 different pressure and temperature combinations without addition of polymer matrix or softener. 27 It was found by WAXS that higher compaction temperatures led to more extensive melting of 28 fibers with the corresponding reduction of the Herman’s factor reflecting the degree of molecular 29 orientation, while the increase of hot compaction pressure suppressed the melting of fibers within 30 SRCs at a given temperature. X-Ray tomography proved the absence of porosity while polarized 31 light Raman spectroscopy measurements for both longitudinal and perpendicular fiber orienta-32 tions showed qualitatively the anisotropy of SRC samples. SEM revealed that the matrix was 33 formed by interlayers of molten polymer entrapped between fibers in SRCs. Moreover, in situ 34 tensile tests demonstrated the increase of Young’s modulus and tensile strength with increasing 35 temperature.