A smart remote control system includes multiple terminals and a server. Each terminal is accessible by an electronic device through use of a registered account/password set. Upon receipt of an association request and a to-be-associated account/password set, one of the terminals is operable to transmit the to-be-associated account/password set to the server. In turn, the server determines whether the to-be-associated account/password set conforms with one of a plurality of user account/password sets stored therein, and enables the one of the terminals to be accessible by the electronic device through use of the to-be-associated account/password set when the determination is affirmative.