In this research work, an attempt has been made to investigate the possibility of wool dyeing with natural dye extracted from the Cinnamomum camphora middle aged/mature leaves. Visually, a range of ecofriendly shades with quite different color gamut of varying hue and tone were produced via the application of different natural mordants. The effect of various natural mordants (gallnut, pomegranate peel, arjun bark, chlorophyll extract, and citric acid) and some commonly used metal mordants (ferrous sulfate, copper sulfate, stannous chloride, and sodium dichromate) on color and fastness properties of dyed wool samples was comparatively evaluated in conjunction with 50% (o.w.f.) of C. camphora natural dye. Dyeing experiments were performed with and without mordants employing pre-mordanting technique. The color of dyed wool fibers were investigated in terms of CIELab (L*, a*, and b*) and color strength values (K/S); and fastness properties were determined as per ISO standard test methods. In general, pre-biomordanted wool fibers with P. granatum (3, 4 and 5% o.w.f.), citric acid (5% o.w.f.) and chlorophyll extract (10–50% o.w.f.) showed comparable color and fastness results compared to those of metal treated samples. Durability of color was also checked to assess the effect of washing of dyed wool fibers. This research work on the use of ecofriendly biomordants will provide a valuable reference in future for ecological and environmentally safe dyeing.