The exposures and work activities of 41 applicators in North Carolina using chlorpyrifos-containing termiticides were characterized. Personal air and urine samples were collected on multiple days within one week. Detailed information about chemical use, tasks, personal protective equipment and hygiene was recorded. During the 202 applicator-days monitored, 415 treatment jobs were performed. Full-shift chlorpyrifos exposures ranged from <0.048 to 110 μg/m3 (N=184), with a geometric mean (GM) of 10 μg/m3. Urinary 3,5,6-trichloro-2-pyridinol (TCP) levels ranged from 9.42 to 1960 μg/g creatinine (N=271) and varied significantly by day of the week (GM range: 169–262 μg/g creatinine). Predictive models for chlorpyrifos air exposure and urinary TCP levels were developed using mixed-effects stepwise linear regression. Determinants of airborne chlorpyrifos exposure included minutes chlorpyrifos applied and enclosed crawl space treated (yes/no). Determinants of TCP levels (depending on the model) included day-of-the-week, the chlorpyrifos air concentration one and two days before urine collection, minutes of chlorpyrifos applied one and two days before urine collection, enclosed crawl space treated (yes/no), and commercial structure treated (time-weighted). Within- and between-worker variablity was similar for airborne chlorpyrifos; however, for TCP, between-worker variability exceeded within-worker variability by six times. The elimination half-life of TCP (26.9 h) and possibly the short sampling interval (one week) may explain the low TCP within-worker variability. Applicators' weekly mean ln(TCP levels) and weekly mean ln(chlorpyrifos air concentrations) were highly and positively linearly correlated (r2=0.73, P<0.0001). In summary, mixed-effects models were successfully constructed to predict airborne chlorpyrifos exposure and urinary TCP levels.