Atomic force microscopy (AFM) measurements of dihedral angles are conducted for the first time to characterize the ratio of the twin-boundary energy (γΤ) to the surface free energy (γS). In plane, twin morphology is measured with AFM, verified by scanning electron microscopy, optical microscopy, and found to be consistent. The chemical composition and homogeneity of annealed Cu10 wt%Zn sample are confirmed by energy-dispersive spectroscopy. AFM data indicate that the average depth and height of the grooves and peaks are 118 ± 45 and 158 ± 45 nm, respectively. Surface roughness parameters, Sq and Sa, are measured by a factor of two to four less than the depth and height of the twin boundaries. Both surface roughness parameters are less with no planar defects present compared with selected areas containing twin boundaries. The average dihedral angle is found to be 167 ± 5° for the grooves and 193 ± 4° for the peaks. The twin to surface interfacial free energy ratio, γT/γS, is 0.0018. The comparison of AFM-based results to the other method-based results obtained on pure metals is discussed.