The unique nonparallel chain arrangement in the orthorhombic γ-form lamellae of isotactic polypropylene (iPP) results in the enhancement of the mechanical properties of γ-iPP. Our study aimed at the investigation of the mechanical properties of γ-iPP nanocomposites with 1-5 wt.% multiwall carbon nanotubes (MWCNT) and 5 wt.% organo-modified montmorillonite prepared by melt-mixing and high-pressure crystallization. Neat iPP and the nanocomposites were crystallized under high pressures of 200 MPa and 300 MPa, and for comparison under 1.4 MPa, in a custom-built high-pressure cell. The structure of the materials was studied using WAXS, SAXS, DSC, and SEM, whereas their mechanical properties were tested in plane-strain compression. Under a small pressure of 1.4 MPa, polymer matrix in all materials crystallized predominantly in the α-form, the most common monoclinic form of iPP, whereas under high pressure it crystallized in the γ-form. This caused a significant increase in the elastic modulus, yield stress, and stress at break. Moreover, due to the presence of MWCNT, these parameters of the nanocomposites exceeded those of the neat polymer. As a result, a 60-70% increase in the elastic modulus, yield stress, and stress at break was achieved by filling of iPP with MWCNT and high-pressure crystallization.