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Mental workload is a critical factor in the use of lower-limb exoskeletons, where motor demands interact with attentional and working memory processes. Eye-tracking has emerged as a non-invasive method, yet its application in exoskeleton-assisted walking remains underexplored. In this study, five healthy participants performed N-back working memory tasks under four conditions: seated-pre, walking without exoskeleton, walking with exoskeleton, and seated-post, across multiple N-back levels (baseline, 0-back, 1-back, 2-back). Eye-tracking data were collected to measure pupil dilation, saccadic dynamics, microsaccades, and blink rate. Linear Mixed Models showed that mean pupil diameter increased by 0.30 mm during walking with the exoskeleton relative to seated baseline (p < 0.01) and by 0.10 mm relative to walking without exoskeleton (p < 0.05), with additional increases of 0.025–0.05 mm per N-back level. Saccade latency increased by ~20 ms with exoskeleton use and 5–15 ms per N-back level, while saccadic amplitude, velocity, and blink rate decreased under high-demand conditions. Microsaccade rate increased by 0.02–0.03 /s during walking with the exoskeleton. These results indicate that pupil dilation and oculomotor adjustments can provide reliable, quantifiable markers of cognitive load during exoskeleton-assisted walking.