The bumper contract win, which includes production of 34.5m information leaflets, 37.5m questionnaires and 64.5m envelopes, follows Polestar's £100m contract renewal with IPC Media, announced last week.
Polestar, which was awarded around £2.5m worth of print for the 2001 Census, described the 2011 Census as "significantly and sizeably different".
A spokesman said: "In 2001 the contract was for base questionnaire production, which was then hand-delivered by numerators. This time there is a requirement that the product will be mailed out. Therefore there is a requirement to address, fulfil them and mail them.
"It's a fundamentally different fulfilment requirement in terms of scale and complexity."
Polestar's involvement in the contract will be led by Polestar Applied Solutions, while production is likely to be centred around Polestar Chromoworks and Polestar Direct – potentially leading to investment at these sites.
The spokesman said: "It is envisaged that the majority if not all print will be handled by Polestar's manufacturing facilities within the UK.
"The majority of methodology and process requirements are existing, but it will require a level of investment at a number of our facilities to make the most of the latest technologies."
Polestar is currently carrying out planning and testing for a rehearsal event next year, which will act as a trial ahead of the main print run in 2010.
Lockheed Martin UK led the consortium, which also included Royal Mail, Cable & Wireless, Logica, Oracle, UK Data Capture, BSS and Steria.
Polestar wins share of £150m 2011 Census bumper contract
A consortium including commercial print giant Polestar has won a £150m contract to support the delivery of the 2011 Census for England, Wales and Northern Ireland.