The operation led to the safeguarding of 400 children and has resulted in charges brought ranging from possessing indecent images of children to serious sexual assault, it said in a statement.
Some 45 police forces across England, Scotland, Wales and Northern Ireland were involved in the operation.
Britain has been rocked by a series of pedophile scandals in the last two years, since revelations that late BBC television host Jimmy Savile was a serial sex offender.
The government recently launched a major inquiry into claims of an alleged parliamentary abuse ring.
The NCA stressed that none of those arrested in the operation is a serving or former MP or member of the government.
"This is the first time the UK has had the capability to coordinate a single targeted operation of this nature," said NCA Deputy Director General Phil Gormley.
Some of those arrested in the NCA operation had unsupervised access to children in the course of their work, including scout leaders and former police officers.
Thirty-nine of those detained had previously come to the attention of police.
"Our aim was to protect children who were victims of, or might be at risk of, sexual exploitation," added Gormley.
"A child is victimised not only when they are abused and an image is taken. They are re-victimised every time that image is viewed by someone," he added.
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