Initially your team can add connections to any Salesforce production, developer or sandbox org. However, as a team owner, you can ensure that team members can only connect to defined Salesforce orgs in Gearset.

This is achieved by specifying which Salesforce My Domains your team are allowed to use when they are adding an org connection.

Configure restrictions in the Connected Services section of the Team Security page:

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Here you can use the edit icons on the right-hand side to bring up a dialog box that allows you to configure restrictions for Production/Developer orgs and Sandbox orgs:

Otherwise, enter the domains of organizations that you want to allow your team to connect to. You can enter just the My Domain name or the entire My Domain URL, and can use * and ? to match any number of characters or any single character respectively (for example, gearset--* will match gearset--sandbox1, gearset--test etc. and gearset? will match gearset1, gearset2 etc.).
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If you don't want to allow any connection at all to the selected type of org (Production/Developer or Sandbox), you can simply turn off the Connections are allowed slider.

To reset to no restrictions, clear all domain names from the input box:

Once you have configured restrictions, your team will only be able to add new connections to Salesforce orgs that match the restrictions you have set. In addition, existing saved connections that do not match the restrictions will be hidden and unavailable for use with new jobs.