Smokefree street policies are relatively rare, and little has been published on the methods for establishing an evidence base to inform such policy making. We aimed to (a) pilot methods for such data collection in New Zealand, a country where local governments are actively pursuing outdoor smokefree policies and (a) to provide data on smoking behavior, attitudes toward smokefree policies, and levels of smoke exposure on streets in Wellington. Three methods were piloted: (a) systematic observation of smoking behavior by observers walking a standard route of major streets, the "Golden Mile" (GM) in Wellington (n = 42 observation runs); (b) measurement of fine particulate levels (PM(2.5)) along this route and with purposeful sampling in selected settings; and (c) an attitudinal survey of pedestrians along sections of this route. Each of the 3 methods proved to be feasible in this urban setting. A total of 932 smokers were observed during 21 hr of observation, an average of 7 smokers every 10 min of walking. Air monitoring indicated fine particulate exposure. Levels of (mean) PM(2.5) were 1.5 times higher during periods when smoking was observed than when they were not (9.3 vs. 6.3 μg/m(3), p = .002). Dose-response patterns were observed for smoking proximity and for smoker numbers. Surveying pedestrians (n = 220) with a brief questionnaire achieved an 81% response rate and was able to identify variation in support for a smokefree GM by different groups (overall support was 55.9%, 95% CI = 49.3%-62.4%). Reasons for support were also identified, for example, perceived health hazards, at 34.1%, was the main reason. These methods can provide information that may contribute to the smokefree streets policymaking process and may also be relevant to informing other smokefree outdoor policies.