And £13 million from the UK aid budget was also be spent educating 100,000 kids in a counter-radicalisation bid.
Downing Street hopes the assistance will also better protect the UK from terror threats while also saving the lives of soldiers and civilians living in Nigeria.
The terror group has killed more than 20,000 people and forced hundreds of thousands to flee their homes.
Mrs May faced questions about the decision to increase support despite Amnesty International raising allegations about Nigerian soldiers raping women rescued from Boko Haram.
The PM told reporters she raised the issue of human rights with president Buhari, adding she welcomed his decision to establish an inquiry to examine the allegations.
The deal includes training to counter improvised explosive devices and developing the Nigerian government's procedures to respond to terror attacks, and aiding Nigeria in the propaganda war.
Nigerian army units will also be trained as a whole rather than individually by the UK before their deployment.
Mrs May arrived in Nigeria on day two of her whistle-stop Africa tour with trade and efforts to combat people trafficking also on the agenda.
Rain started to fall as Mrs May left the RAF Voyager and after a military reception, she resisted the temptation to dance for a second day when greeted by dancers and drummers at the airport in Abuja.
She travelled to the presidential villa for talks with president Buhari, amid a chaotic media scrum on the red carpet.
Mrs May later travelled to Lagos to announce business projects, develop financial links amid post-Brexit uncertainty for the City of London, and meet survivors of modern slavery.
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