Introduction: Negative air ions (NAIs) are beneficial in improving memory, anti-depressant effects, productivity, psychological health, and well-being by inducing alkalinity in the body. Cerebral Palsy (CP) is a neurological disorder that impairs movement and elicits behavioral issues like anxiety, anger, agitation, dependency on others, hyperactivity, incompatibility, and stubbornness. Such behaviors may hamper their cooperation or willingness for physiotherapy. Methodology: Evidence-based studies to support that NAIs can augment the rehabilitation of CP are scant so, the present study was designed to determine if exposure to NAIs can normalize behaviors and physical outcomes. Ethical approval was taken from IBC, University of Karachi followed by the consent of the participants and the Al Umeed Rehabilitation Association where the intervention study was conducted in 2021. CP-inflicted participants were randomly allocated to the control and intervention groups. Both groups continued their regular twice-a-week physiotherapy sessions, but the intervention group also received 40-minute exposure to 10000 negative ions/cm3 for 6 weeks. Outcomes were assessed using a researcher-designed physiotherapist reporting questionnaire and Modified Ashworth Scale. Results: Analysis using SPSS v.28 demonstrated significant improvement in calmness, cooperation, physical condition, and willingness for physiotherapy along with minimal alleviation of spasticity. The possible role of neuronal pathways, synaptic response, and neurotransmitters such as acetylcholine, dopamine, gamma-aminobutyric acid, and serotonin have been discussed. Conclusion: The study concludes that NAIs may alleviate spasticity and normalize behaviors during physiotherapy sessions. We suggest the inclusion of this novel intervention in the multidisciplinary rehabilitation plan after going through the second and third-phase clinical trials.