This paper, with the use of data from the SHRP 2 naturalistic driving study, provides a preliminary evaluation of the effectiveness of high-visibility crosswalks (HVCs) in improving pedestrian safety at un-controlled locations. This evaluation was accomplished by analyzing the driving behavior of SHRP 2 participants at three uncontrolled locations at the Erie County, New York, test site. In this context, crash surrogates (i.e., speed, acceleration, throttle pedal actuation, and brake application) were used to evaluate the participants’ driving behavior, primarily on the basis of data from before and after the HVC installation. The before–after analysis allowed the assessment of HVC effectiveness in driver behavior modification. Mixed logit and random parameters linear regression models were estimated, and panel effects and unobserved heterogeneity were accounted for. Several factors were explored and controlled for (e.g., vehicle and driver characteristics, roadside environment, weather conditions), and the preliminary exploratory results show that HVCs can improve pedestrian safety and positively modify driving behavior.