Step 1: Rewrite:
$(a + b)^2 - c^2 = ab$ means $c^2 = a^2 + ab + b^2$.
Step 2: Compare with cosine rule:
$c^2 = a^2 + b^2 - 2ab\cos C$, so $-2\cos C = 1$, giving $\cos C = -\frac12$ and $C = 120^{\circ} = \frac{2\pi}{3}$.
Final Answer:
The angle is $\frac{2\pi}{3}$, option (B).
\[ \boxed{\frac{2\pi}{3}} \]