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Pimelic acid (PA) is used as a new surface modifier for mica (MC). The effects of PA treatment on the crystallization, morphology, and mechanical properties of isotactic polypropylene (iPP)/MC composites have been investigated. FTIR analysis reveals that PA reacted with phlogopite MC, and pimelates are formed during the treatment. The results of wide angle X-ray diffraction, differential scanning calorimetry, and polarized light microscopy prove that PA-treated MC induces a large amount of b-iPP and decreases the spherulite size of iPP. The results of SEM show that PA treatment improves the orientation and dispersion of MC plates in the matrix. The notched impact strength of the composites is improved dramatically by PA-treated MC. The superior toughness is ascribed to the more ductile b spherulites, preferential orientation of MC plates, small spherulite size, and improved dispersion of MC plates in the matrix.