The as-yet-untitled autobiography is set for release in 2023 and is expected to touch on his childhood and early political career as well as his tumultuous four years as Donald Trump's right-hand man.
Pence's agent, David Vigliano, claimed the deal was worth "well into seven figures," The Associated Press reported, while CNN suggested he could be paid up to $4m.
"I am grateful to have the opportunity to tell the story of my life in public service to the American people, from serving in Congress, to the Indiana Governor's office and as Vice President of the United States," Pence said in a statement.
"I look forward to working with the outstanding team at Simon & Schuster to invite readers on a journey from a small town in Indiana to Washington, D.C."
So what can readers expect from the book?
Lifting lid on four years in Trump's White House
The main draw for many will be the untold stories from the heart of what critics called an often-dysfunctional Trump administration.
Pence remained loyal to his former boss throughout his tenure, avoiding the fate of many others who were dismissed over the four years, suggesting he has a better idea than most about the hirings and firings, controversies and decision making that defined the Trump presidency, including the government's reaction to the first year of the coronavirus pandemic.
And Pence is the first senior official from within the Trump team to have announced a deal since the administration was replaced in January.
If other political memoirs are anything to go by, Pence's book may well offer tantalizing details of his time in office.
Will Pence heal rifts or deepen them?
The siege of the US Capitol on January 6 by Trump's supporters led to a partial fracturing of the Republican base.
Pence was at the heart of that since he angered Trump loyalists by refusing demands that he help overturn the election results, and relations between the two men were said to be fraught in the final days of the presidency.
Trump and his supporters were strongly critical of Pence for not intervening, with some of those who rioted at the Capitol chanting "Hang Mike Pence."
It will be interesting to see if the book attempts to heal those divisions or deepens them further.
2024 presidential run
Tied to talk of divisions within the Republican base are rumours of a possible 2024 presidential bid.
Pence has long been touted as a potential candidate and his reemergence into the public eye in recent weeks has fueled speculation of a bid for the White House.
According to YouGov Ratings, he is the fourth most famous Republican, per data collected between October and December last year.
But he will face opposition from those further on the right of the party, who favor a return of Trump.
Infowars conspiracy theorist Alex Jones told his 178,000 followers on Gab that Pence was mulling a run after "betraying constitution, Trump, the American people."
Details of Pence's conservative advocacy group
The book should shed more light on Pence's political activity since leaving Washington.
The former vice president recently launched his new Advancing American Freedom organization, which will "merge traditional conservative values with the Make America Great Again policy agenda."
The autobiography may give more details about this and other political advocacy work he has planned, with the former vice president having already joined Heritage Foundation, a conservative Washington-based think tank.
Could Trump get a book deal?
Confirmation that major book publisher Simon & Schuster has agreed a two-book deal for the former vice president could pave the way for Trump to secure his own agreement.
However publishers are said to have largely shied away from agreeing to work with the former president for fear of reputational damage and a backlash from readers, authors and employees in the context of the deadly Capitol riots, which Trump is accused of inciting.
