Mr Matheson made the calls to the UK Government as he travelled to The Hague on Friday to meet Rob Wainwright, director for Europol to see first-hand the work of the UK Liaison Bureau, including the role played by Police Scotland’s seconded officer.
Europol, the EU’s law enforcement agency headquartered in the Netherlands assists member states to carry out over 18,000 cross-border investigations every year involving serious international crime and terrorism.
The agency is currently engaged in on-going activity to support policing operations in Scotland such as targeted pan-European housebreaking, human trafficking, child sexual exploitation and cyber crime.
Under current EU opt-in arrangements, the UK Government must indicate by January 2017 if it is to accept a new regulation on Europol - failure to do so would mean the UK will no longer be a member of the framework from May 2017.
Mr Matheson said: “The ability to share information quickly and co-ordinate operations with other law enforcement agencies through Europol is key to detecting, disrupting and detaining criminals across borders.
“That is necessary to keep Scotland and the rest of the UK safer from the threats of organised crime, cybercrime and terrorism.
“Europol supports the effective operation of the European Arrest Warrant through which Police Scotland has arrested 301 offenders, while 43 offenders have been returned to Scotland to face justice.
“European co-operation also gives our police practical support and expertise from the European Cybercrime Centre (EC3), and enhances their ability to locate missing persons, as well as tracking down fugitives.
“As the Home Secretary said recently, Europol has played an important role in keeping us safe. That is why I have written to her, pressing for the UK Government to end the uncertainty for our police and their law enforcement partners by making a decision to sign up to the revised Europol arrangements.”