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The men, aged 18 and 22, were arrested on Saturday, April 18, on suspicion of possessing a firearm with intent to cause fear of violence.
The arrests follow an incident on Park Road in Barry on Monday, April 13, at around 10.30pm.
Police had received reports of loud bangs and an assault.
An 18-year-old from Llanrumney has already been charged and remains in custody.
A 17-year-old from Canton remains on police bail.
Enquiries remain ongoing.
