Tefillin is mentioned twice in the passage about Exodus from Egypt:
And it shall be for a sign for you upon your hand, and for a memorial between your eyes, that the law of the LORD may be in your mouth; for with a strong hand did the LORD bring you out of Egypt.
And it shall be for a sign upon your hand, and as totafot between your eyes; for with a mighty hand did the LORD bring us forth out of Egypt.
and twice in the shema passages:
And you shall bind them as a sign upon your arm, and they shall be as totafot between your eyes.
You shall put these words of mine on your heart and on your soul; and you shall tie them for a sign upon your arm, and they shall be as totafot between your eyes.