Aims To assess the feasibility and effectiveness of a new service using referral liaison advisers to increase the number of referrals of parents/carers at selected Children's Centres to National Health Service (NHS) Stop Smoking Services (SSS) and/or smoke-free families schemes (SFS). Design This mixed-methods pilot study collected numerical data on indicators of smoking behaviours and carried out face-to-face and telephone interviews. Settings Thirteen Children's Centres in Liverpool and Nottingham using local providers of smoking cessation services, from September 2010 to April 2011. Participants Parents and carers registered with, and staff working for, Children's Centres. Measures Number of smokers referred to smoking cessation services and/or smoke-free family schemes and the views of service providers and users on the new service. Findings In Liverpool, 181 referrals to NHS SSS were made from 331 identified smokers (54.7%); extrapolated to 12 months, this represents a 182% increase in referrals from baseline and a similar extrapolation indicates a 643% increase from baseline of referrals to smoke-free families schemes. There were no reliable baseline data for Nottingham; 31 referrals were made (30.7% of smokers) to SSS and 44 referrals to SFS from 52 contacts (84.6%). The interviews highlighted the need for sustained personal contact with parents/carers to discuss smoking behaviours and concerns and their willingness to be referred to SFS as part of caring for their child. Conclusions Routine recording of smoking status and appropriate follow-up by trained staff in Children's Centres can lead to significant numbers of clients attending stop-smoking services, although relatively few stop smoking.