Despite the recently increasing research interest, this is one of the first studies employing a panel sample of users and nonusers to understand the bike-sharing phenomenon ( = 205). On the basis of a novel surveying technique, a case study on the clients of the state-of-the-art bike-sharing scheme of Madrid (Spain) is presented. BiciMAD is a system of the latest generation, namely, multimodal demand responsive bike-sharing: a fleet of electric pedal-assisted bicycles (pedelecs) with an advanced technology and unique smart service configuration to tackle challenges that may hinder the promotion of cycling and bike-sharing in the city. A statistical test has verified that there is a moderate association between previous intention and actual use of bike-sharing (Cramer's V = 0.25) and both barriers and motivators of further use have been identified. Indicators on mobility patterns show that although drawing primarily from other sustainable modes of transport, bike-sharing has increased mobility (total number and distance of trips) and especially active travel but decreased the perceived travel time.