What isosceles triangle meets the following requirement:
- the unique side has a length of 1
- the unique angle can be multiplied by a whole number to equal 180°
- the similar side lengths are whole numbers
- the triangle is not equilateral
If it is possible and there are multiple, what is the triangle with the greatest unique angle?
You wrote two conditions for the unique side length. I assume you meant that length to be $1$, and the equal sides to be of integer length.
Let the unique angle be $2\varphi$ so you can easily split the triangle into two congruent right-angled triangles. Then the ratio between half the unique side length and the equal side length $a$ is
$$\sin\varphi=\frac{\,\frac12\,}a\quad\Rightarrow\quad\csc\varphi=2a$$
Now consider Niven's theorem. It states that
$$\sin\varphi=x\text{ with } \varphi\in\pi\mathbb Q,x\in\mathbb Q,0\le\varphi\le90° \\\Rightarrow\quad (\varphi,x)\in\{(0°,0),(30°,\tfrac12),(90°,1)\}$$
So simply from the fact that your solution would have to satisfy both $\varphi\in\pi\mathbb Q$ and $\sin\varphi=\tfrac1{2a}\in\mathbb Q$ along with $0<\varphi<90°$ you can see that there can be no solution satisfying the requirements.