Human movement requires an ongoing, finely tuned interaction between muscular and tendinous tissues, so changes in the properties of either tissue could have important functional consequences. One condition that alters the functional demands placed on lower limb muscle-tendon units is the use of high-heeled shoes (HH), which force the foot into a plantarflexed position. Long-term HH use has been found to shorten medial gastrocnemius muscle fascicles and increase Achilles tendon stiffness, but the consequences of these changes for locomotor muscle-tendon function are unknown. This study examined the effects of habitual HH use on the neuromechanical behavior of triceps surae muscles during walking. The study population consisted of 9 habitual high heel wearers who had worn shoes with a minimum heel height of 5 cm at least 40 h/wk for a minimum of 2 yr, and 10 control participants who habitually wore heels for less than 10 h/wk. Participants walked at a self-selected speed over level ground while ground reaction forces, ankle and knee joint kinematics, lower limb muscle activity, and gastrocnemius fascicle length data were acquired. In long-term HH wearers, walking in HH resulted in substantial increases in muscle fascicle strains and muscle activation during the stance phase compared with barefoot walking. The results suggest that long-term high heel use may compromise muscle efficiency in walking and are consistent with reports that HH wearers often experience discomfort and muscle fatigue. Long-term HH use may also increase the risk of strain injuries.