This is a follow-up of this question.
Let $\psi:[0,\infty) \to [0,\infty)$ be a strictly increasing $C^2$ (or $C^{\infty}$) function, satisfying $\psi(0)=0$.
Suppose that the function $f(r)=\psi'(r)+\frac{\psi(r)}{r}$ is non-increasing.
Must $\psi$ be concave?
The converse statement is true, i.e. $\psi$ concave implies $f$ non-increasing: Indeed, $$ f'(r)=\psi''(r)+\frac{1}{r}(\psi'(r)-\frac{\psi(r)}{r}), $$ $\psi'' \le 0$ by concavity, and since $\psi(r)=\int_0^r \psi'(t)dt \ge \int_0^r \psi'(r)dt=r\psi'(r)$, the term $\frac{1}{r}(\psi'(r)-\frac{\psi(r)}{r})$ is also non-positive.
Edit:
Here is a partial result-I can prove that $\psi''(0) \le 0$.
By our assumption $$ 0 \ge f'(r)=\psi''(r)+\frac{1}{r}(\psi'(r)-\frac{\psi(r)}{r}), $$ for every $r>0$. Using the mean value theorem (twice), we can rewrite this as $$ f'(r)=\psi''(r)+\psi''(s(r)) \le 0, \tag{1} $$ where $s(r)$ is some point in $(0,r)$.
In particular, taking the limit when $r \to 0$, we deduce that $\psi''(0) \le 0$.