Is it possible to apply an On/Off schedule to an entire VRF system in OS or does this have to be done terminal-by-terminal?

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The AirConditioner:VariableRefrigerantFlow system object has an availability schedule field.

"This alpha field defines the name of the schedule (ref: Schedule) that denotes whether the heat pump operates during a given time period. A schedule value equal to 0 denotes that the heat pump must be off for that time period. A value other than 0 denotes that the heat pump is available to operate during that time period. This schedule may be used to completely disable the heat pump (and all of its terminal units) as required. If this field is blank, the unit is enabled the entire simulation."

You can set it in the OpenStudio app in the HVAC systems tab under the VRF system dropdown and clicking on the VRF system object.