The understanding of biomechanical deficits and impaired neural control of gait after stroke is crucial to prescribe effective customized treatments aimed at improving walking function. Instrumented gait analysis has been increasingly integrated into the clinical practice to enhance precision and inter-rater reliability for the assessment of pathological gait. On the other hand, the analysis of muscle synergies has gained relevance as a novel tool to describe the neural control of walking. Since muscle synergies and gait analysis capture different but equally important aspects of walking, we hypothesized that their combination can improve the current clinical tools for the assessment of walking performance. To test this hypothesis, we performed a complete bilateral, lower limb biomechanical and muscle synergies analysis on nine poststroke hemiparetic patients during overground walking. Using stepwise multiple regression, we identified a number of kinematic, kinetic, spatiotemporal and synergy-related features from the paretic and non-paretic side that, combined together, allow to predict impaired walking function better than the Fugl-Meyer Assessment score. These variables were time of peak knee flexion, VAFtotal values, duration of stance phase, peak of paretic propulsion and range of hip flexion. Since these five variables describe important biomechanical and neural control features underlying walking deficits poststroke, they may be feasible to drive customized rehabilitation therapies aimed to improve walking function. This paper demonstrates the feasibility of combining biomechanical and neural-related measures to assess locomotion performance in neurologically injured individuals.