Using the digits 0 to 9

Supplementary Angles:
[tex]\boxed{100°} and \boxed{80°}[/tex]
Arithmetically speaking, the closest 2 supplementary angles can get (in 3 and 2 digits respectively) is the upwritten.
Complementary Angles:
[tex]\boxed{45°} and \boxed{45°}[/tex]
Simply, in this case, for angles to be numerically as close as possible - make both the angles 45°.