The 30-year-old man was tracked down in local woods following reports that items were being thrown into the grounds of Erlestoke Prison.
Police Dog Conan and his handler detained the suspect after a brief search of a nearby wooded area.
He was arrested by colleagues from Wiltshire Police's armed response unit on suspicion of conveyance of prohibited articles into the prison.
A vehicle believed to have transported the suspect the location was stopped by the Community Policing Team in Salisbury.
A 30-year-old man and 31-year-old woman were arrested on suspicion of conveyance of prohibited articles into prison. The man was also arrested on suspicion of drug-driving.
Sgt Paul Harvey said: "These arrests came about as a result of an effective and coordinated response by my colleagues, including PD Conan and his handler who tracked the initial suspect under challenging circumstances.
"Officers worked together seamlessly in response to the initial call and we are pleased to have arrested and detained three suspects in relation to this incident."