Old age brings unique challenges, and in India, many senior citizens in old-age care homes face loneliness, social isolation, and reduced autonomy—factors that raise the risk of depression and anxiety. The living environment plays a crucial role in Older Adults mental health, while spirituality can offer significant support and resilience. This cross-sectional study in the Delhi-NCR area included 120 Older Adults participants, with 60 from old age homes and 60 from their natural home environments. The Depression, Anxiety, and Stress Scale (DASS) was used to evaluate mental health, while the Spirituality Attitude Scale (SAS) measured spirituality. Participants in old age homes (n = 60) had a mean age of 76.36 ± 6.43 years, while those living in natural settings (n = 60) had a mean age of 72.2 ± 8.09 years. Relationship maintenance scores were significantly lower in old age homes (30.41 ± 7.47) compared to natural home settings (39.28 ± 11.74), with a p-value of < 0.001. Similarly, the total spirituality scores showed significant differences: residents in old age homes had a mean score of 34.04 ± 8.31, while those in natural home settings scored 41.63 ± 9.80 (p < 0.002). Older Adults individuals in natural home settings demonstrate higher spirituality scores compared to those in old age care homes, suggesting a link between living environment and spiritual well-being. This highlights the need to consider environmental factors when exploring the relationship between spirituality and mental health in the Older Adults.