Across England and Wales, more certificates for firearm and shotgun users were removed last year than ever before, which campaign group Action on Armed Violence said "can only be good".
The Gun Control Network called on the Government to "dramatically increase" licence fees so the police can conduct more thorough checks.
Home Office figures show 111 shotgun certificates were revoked by Devon and Cornwall Police in the year to March – up from 73 the year before, and the highest figure since comparable records began in 2008-09.
The figures also show 52 firearm licences were revoked over the same period – up from 37 in 2022-23, and also the highest figure since comparable records began in 2008-09.
The police can revoke any individual's firearms licence if they believe they cannot be trusted with it, are a danger to the public, or no longer have a good reason to hold it.
Nationally, 1,559 shotgun certificates were revoked across England and Wales – a 34% increase on 2022-23, and the highest figure since comparable records began in 2008-09.
Meanwhile, firearm revocations also reached record levels, rising by 21% to 507.
Dr Iain Overton, executive director at Action on Armed Violence, said gun control has repeatedly reduced death tolls globally.
He added: "The recent revocation of these shotgun and other licenses may have complex and individual reasons, such as concern for suicidal intention amongst economically-hit farmers, but in so doing they further reduce the likelihood of guns being used to murder or self-harm. This can only be good."
A spokesperson for the Gun Control Network said there have been six shootings in Great Britain where three or more people have died in the last 14 years, five of which were committed by licensed gun owners.
They added: "Clearly our firearms licensing process is broken, and many bereaved and traumatised families are suffering the consequences.
"The licence fees need to increase dramatically so the police have more funding to conduct more thorough checks."
The data also shows 25,871 shotgun and 10,164 firearm certificates were active in Devon and Cornwall as of the end of March, the equivalent of 3,649 and 2,110 per 100,000 people respectively.
The British Association for Shooting and Conservation said the police are increasingly "depriving perfectly safe people of their certificates and leaving it to the court to make the final decision".
Director of firearms Bill Harriman questioned the consistency of police forces' administration of licences following the coronavirus pandemic, adding the barriers for a "safe and responsible person" to get involved are "becoming increasingly insurmountable".