Background: Alzheimer’s disease has become increasingly prevalent among the older population, leading to significant social and economic burdens. Transcranial photobiomodulation (tPBM) has shown promise as a cognitive intervention for enhancing cognitive efficiency in healthy older adults, and individuals with mild cognitive impairment and Alzheimer’s disease. However, determining the optimal tPBM dosage is crucial for ensuring effective and efficient intervention. Objective: This study aimed to compare the effects of different dosages in a single tPBM session on cognitive efficiency in healthy older adults. Methods: In this randomized controlled trial, 88 healthy older participants were assigned to either a single dose (irradiance = 30 mW/cm2, fluence = 10.8 J/cm2; n = 44) or a double dose (irradiance = 30 mW/cm2, fluence = 21.6 J/cm2; n = 44) tPBM session. Cognitive efficiency was assessed using functional near-infrared spectroscopy during a visual working memory span task. Results: The single dose group exhibited significantly greater cognitive efficiency enhancement, indicated by a more pronounced reduction in oxygenated hemoglobin during a challenging task level (span level 9) (p = 0.021, d = 0.50), and better working memory task performance (p = 0.045, d = 0.31). Furthermore, participants with better visuospatial abilities demonstrated greater improvement after a single dose (r = –0.42, p = 0.004). In contrast, participants with varying cognitive function did not exhibit additional benefits from a double dose (r = –0.22–0.15, p = 0.16–0.95). Conclusions: These findings suggest that higher tPBM dosages may not necessarily result in superior cognitive improvement in older adults.