Your reasoning is a sequence of logical consequences (and not equivalences) that lead you to conclude that $\theta\in \{69.2, \,110.8, \,212.3, \,327.7\}:=S$.
You don't necessarily know that every $\theta \in S$ will satisfy the initial equation, you just know that every solution to the equation will be in $S$.
In fact it doesn't happen that every element of $S$ will be a solution to the equation. Note that for every $\theta\in S$ we have $2-\sin (\theta)>0$. However you can check that not all $\theta\in S$ will make the inequality $3\cos (\theta)>0$ true.
The reason for all this was that you squared the equation. Note that $2^2=(-2)^2$ and $2\neq -2$.
As an example of a similar problem consider the equation $\cos (\theta)=\sin (\theta)$ in $[0,360]$. You should know that the solutions to this equation are $45º$ and $225º$. However if you proceed in a similar way you get
$$\cos (\theta)=\sin (\theta) \Longrightarrow (\cos (\theta))^2=(\sin (\theta))^2 \Longrightarrow \theta \in \{45º, 135º, 225º, 315º\}$$
You can "go forward" in your reasoning, but you can't "go backwards".