Four years later, fears have grown that the money has been frittered away, with around a third spent on teachers' back pay. But, undeterred, Mr Zuckerberg recently announced that he would donate a further $120 million (pound;71 million) to improve schools in the San Francisco Bay area.
His forays into the school reform agenda are part of a growing movement among tech billionaires in the US, who want to change the country's school system and are willing to put their money where their mouths are. It is a group referred to by education academic and campaigner Diane Ravitch as the "billionaire boys' club".
Microsoft founder Bill Gates, via his charity the Bill and Melinda Gates Foundation, effectively bankrolled the Common Core State Standards - the country's first attempt to introduce national standards - with $200 million (pound;119 million) in donations.
Reed Hastings, chief executive of video-streaming website Netflix, has set up his own chain of charter schools, Rocketship Education, on the East and West Coasts.
And last week David Welch, another Silicon Valley entrepreneur who made millions in fibre-optic technology, funded a lawsuit to see "teacher tenure" laws overturned - a case that has huge ramifications for the rest of the US. A Los Angeles County Superior Court judge ruled that laws preventing teachers from being fired, along with "last in, first out" policies that keep longer-serving teachers in jobs regardless of their performance, were "unconstitutional".
Similar lawsuits could now be filed in around half the US states where teacher tenure laws are still in place, effectively ending long-standing job-protection laws.
The involvement of Silicon Valley's wealthiest in education has been welcomed by reformers all the way to the White House, with education secretary Arne Duncan praising the landmark court ruling and describing it as a "mandate to fix the problems" of the US education system.
But the interventions of the billionaire boys' club are not always successful, as Mr Zuckerberg's early intervention has shown. The $100 million intended for Newark was meant to provide charter schools and a new contract tying teacher bonuses to student performance, yet nearly all of it has gone. More than $30 million (pound;18 million) was spent on teachers' back pay, and experts claim that no funding will be left for the bonus scheme.
And according to statistics from Newark's Department of Education, although graduation rates rose from 54 per cent in 2009 to 67 per cent in 2013, test scores in reading and maths have largely flatlined.
To teaching unions in the US, which are among the biggest donors to the Democratic Party, the involvement of tech billionaires in education is an attempt by a small cabal of businessmen to push their own "extreme agenda".
Dennis Van Roekel, president of the National Education Association, the largest union in the US, told TES: "Who do you trust when it comes to deciding what's best for students? Your child's third-grade teacher or a Silicon Valley billionaire who wants to remake education into a business?
"For parents and communities, the answer is simple. Unfortunately, some use philanthropy as a way to push their own agenda. It's time that we put our children's education back in the hands of educators, who only have students' achievement as their agenda."
Although the unions view the entrepreneurs' involvement as a bid to break up and privatise public education, others within the tech industry see it as an effort to fill the skills gap between schools and industry.
Sherry Coutu, a tech entrepreneur and investor in online companies such as LoveFilm and Zoopla who also acts philanthropically in the ed-tech sector, believes the tycoons' motivation is ensuring the future of their companies.
"These people see a huge gap, a vast delta between the skills these kids are coming out of school and college with and the skills we need them to have in our companies," Ms Coutu said. "And if our students made different decisions along the lines of Stem [science, technology, engineering and maths], coding and entrepreneurship, it would be easier for our companies in 10 to 15 years' time to hire these people.
"What's coming out of school is not what these tech companies need. And if these billionaires are still aspiring to own their companies in 10 to 15 years' time - which a Zuckerberg will surely fancy - then you are acting on a problem you know you will have in the years to come."
The business leaders were taking a very "industrial" approach to the education system, Ms Coutu admitted.
"They have almost a product focus [when it comes to schools]," she said, "meaning they see the current outcomes are unacceptable to them and their companies, and also to the long-term growth of the economy. So they want to do something about it. And they have the means to do it."