The use of quantitative methods to analyze the loss in gait smoothness, an increase in movement intermittency which is a distinguishing hallmark of motor deficits in stroke patients, has gained considerable attention in recent years. In the literature, the spectral arc length (SPARC), as well as metrics based on the measurement of the jerk, such as the log dimensionless jerk (LDLJ), are currently employed to assess smoothness. However, the optimal measure for evaluating the smoothness of walking in stroke patients remains unknown. Here, we investigated the smoothness of the body’s center of mass (BCoM) trajectory during gait, using an optoelectronic system, in twenty-two subacute and eight chronic patients before and after a two-month rehabilitation program. The two measures were evaluated for their discriminant validity (ability to differentiate the smoothness of the BCoM trajectory calculated on the cycle of the affected and unaffected limb, and between subacute and chronic patients), validity (correlation with clinical scales), and responsiveness to the intervention. According to our findings, the LDLJ outperformed the SPARC in terms of the examined qualities. Based on data gathered using an optoelectronic system, we recommend using the LDLJ rather than the SPARC to investigate the gait smoothness of stroke patients.