Ligament cross-sectional areas are difficult to determine because ligaments are soft tissues, can be very short, and may be deep between bones. However, accurate measurements are required for determining the material properties from mechanical testing. Many techniques have been tried, but most suffer from one or more of the following: tissue deformation, tissue destruction, submersion of the tissue in saline, the need for a clear line of site, the inability to detect concavities, or poorly defined cross-sectional perimeters. Molding techniques have been used but have been limited by material issues such as large shrinkages, the inability to capture small detail, or the need to destroy the mold to remove the ligament. In this study, we developed a suitable molding and casting technique without systematic shrinkage that could accurately capture the odd shapes and concavities of foot and ankle ligaments with small clearances between bones. Metal rods of 1.62 mm, 2.90 mm, 3.18 mm, and 9.43 mm in diameter were molded using a liquid silicone rubber and cast with polyurethane. The effect of cutting the mold for specimen removal was investigated, and similar tests were done in the presence of saline. Image analysis software was used to determine the cross-sectional areas from photographs of cut castings. In addition, four different ligaments (each ) were dissected, molded, and cast. The cross-sectional area of each ligament was obtained. The maximum difference in area for all cases was 2.00%, with the majority being less than 1.00%; the overall root mean square error was or 0.97%. Neither cutting the mold for specimen removal nor the presence of saline affected the cross-sectional area of the castings. Various representative foot and ankle ligaments were also molded and cast to capture fine detail of the ligament midsubstance including concavities. We have developed a method of measuring ligament cross-sectional area that can overcome the limitations of other area measurement techniques, while accounting for the complicated anatomy of the bones of the foot. The method was validated using metal rods of known diameters, and a representative set foot ligaments was analyzed.