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Direct potentiometric method for determination of penicillamine in pharmaceuticals by using commercial copper ISE is described. Proposed method is very inexpensive, simple and reasonably fast method for determination of Pen in acetic buffer, pH = 4 without pretreatment of pharmaceuticals. Determination is based on the reaction between Pen and Cu2+ from electrode membrane. Described method has linear response range for Pen from 2×10−6 to 1×10−2 mol L−1 with limit of detection of 1.1×10−6 mol L−1. Found concentrations of Pen are in very good agreement with declared ones with standard deviation values in range 4.00−4.50 %.