This really isn't either of those things in the context of DHCP. What you are talking about is usually called a Reservation.
Anyway, here's how to do it. Go into your DHCP scope and click on the Reservations object. On the Action menu, click "new reservation" and fill in the blanks. One of the options you can set is MAC address, which you will use to - you guessed it - assign IP addresses based on MAC address.
To extend this a little bit, if you want to only give out IP addresses to certain MAC addresses, configure your scope in such a way that all addresses are reserved (or excluded). Then create a reservation for each IP address, specifying the desired MAC address.
If you are doing this for security reasons, brian is pretty much right. MAC filtering (a firewall function) can be used to restrict which devices may communicate on your network. DHCP reservations will not prevent undesired devices from communicating on your network. Choose your tools wisely.