Abstract Throughfall and stemflow measurements taken in a mature high elevation red spruce stand, and precipitation measurements made in a nearby clearing, were used to calculate weekly net throughfall (=throughfall + stemflow - precipitation) sulfate deposition and net throughfall volume in the stand over a 20-week period. The study fortuitously was divisible into a low cloudwater deposition period, during which precipitation volumes generally exceeded throughfall volumes, and a high cloud period, during which the reverse was true. Weekly cloudwater deposition volume was estimated independently from continuously recorded cloudwater collections by an artificial tree located on an elevated platform in the clearing. Weekly net throughfall volume correlated well with cloudwater deposition volume ( r = +0.86). Precipitation accounted for only 25% of the throughfall sulfate collected throughout the study and only 15% of that collected during the high cloud period, as net throughfall sulfate was 2.4 times greater during the high cloud period than during the low cloud period. Weekly estimates of cloudwater sulfate deposition correlated well ( r = +0.74) with measures of net throughfall sulfate during the high cloud period. Dry deposition models were used to estimate weekly dry S deposition; weekly estimates of the wash-off of this dry deposition also correlated well ( r = +0.76) with net throughfall sulfate during the low cloud period. During the high cloud period, estimates of cloudwater S plus dry S deposition accounted for 67% of the sulfate collected in net throughfall; however, during the low cloud period only 55% of net throughfall sulfate was accounted for. The low percentage of sulfate accounted for during the low cloud period suggests that the dry models were underestimating S deposition. Possible reasons for underestimation include failure to consider fully topographic complexity and edge effects, underestimates of surface wetness, and the possibility of canopy sources of sulfate (foliar leaching). These results support the use of throughfall sulfate measurements as gross estimates of (1) total S deposition, (2) total dry S deposition (using net throughfall in environments where cloudwater deposition accounts for less than 5% of total sulfate deposition) and/or (3) total cloud S deposition (subtracting precipitation and dry inputs from total throughfall sulfate in high cloud environments).