Contractors Lendlease will build the development in the city centre at Copperas Hill to form a gateway for the Liverpool's Knowledge Quarter.
In addition, it will bring together LJMU's Mount Pleasant and Byrom Street campuses.
The five-floor building will include two mezzanine floors and use of the roof for sports and recreation, increasing the floor area from 280,000 sq.ft. to 355,000 sq.ft.
The development will also house the University's three libraries combined into one facility, as well as student zones, a central teaching unit, sports facilities and a Students' Union.
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Other facilities include a cafe and retail space, a careers centre, student support services, student administration and LJMU's Teaching and Learning Academy.
Lendlease are underway with enabling works on site and will remove the exterior of the former Royal Mail sorting office to expose the internal frame in May.
LJMU Vice-Chancellor, Professor Nigel Weatherill, said: "Sometimes the term 'transformational' is overused but the impact of the new development at Copperas Hill cannot be over-estimated. Importantly for LJMU it will revolutionise the student experience and the physical shape of the University as well as having a highly positive effect on the city itself.
"Here is a structure which lies in a prime, central location of the city, and we are now investing over £100 million to ensure it is successfully regenerated, which will lead to the area once again becoming a hive of activity."
The development is expected to be open for use at the start of the academic year in 2018.
(LM)
