Background/Objectives: This study examined the impact of spasticity-related unpleasant sensations (pain, heaviness, stiffness) on various domains of the International Classification of Functioning, Disability, and Health (ICF) and psychosocial well-being in individuals affected by stroke or traumatic brain injury (TBI). The primary aim is to explore how these sensations affect daily activities, participation, and overall quality of life, guided by the comprehensive framework of the ICF. Methods: Utilizing a secondary analysis of data from a cohort undergoing Botulinum toxin type-A treatment for spasticity post-stroke or TBI, we developed and administered an ad-hoc questionnaire focusing on ICF domains such as body function, activities and participation, and psychosocial aspects such as mood, relationship, social life, motivation, and sleep quality. Spearman rho correlation was applied to assess the relationship between unpleasant sensations and functional as well as psychosocial outcomes among 151 participants. Results: This study identified significant correlations between the severity of unpleasant sensations and limitations in daily functioning, particularly in activities of daily living and mobility. Furthermore, an impactful association was identified between increased unpleasant sensations and deterioration in psychosocial well-being, notably in mood and sleep quality. Conclusions: These findings advocate for a person-centered approach in spasticity management, emphasizing the integration of sensory impairment strategies into rehabilitation to enhance functional outcomes and quality of life. Such an approach aims to improve functional outcomes and enhance the quality of life for individuals experiencing spasticity post-stroke or TBI. Future directions include targeted interventions to alleviate these sensations, support better rehabilitation results and improve patient experiences.