Following the previous indication of Professor Brown I want to add another possible way to see natural transformation which is a generalization of the previous definition.
Given categories $\mathcal C$ and $\mathcal D$ and two functors between them $\mathcal F,\mathcal G \colon \mathcal C \to \mathcal D$ then a natural transformation $\tau$ can be defined as a functor $\tau \colon \mathcal C \to (\mathcal F \downarrow \mathcal G)$ which arrow components are the diagonal functions, sending each arrow $f \in \mathcal C(c,c')$, with $c,c' \in \mathcal C$ to $(f,f) \in (\mathcal F \downarrow \mathcal G)(\tau(c),\tau(c'))$.
Edit: I think the definition of natural transformation proposed by professor Brown probably can be even a more natural than the one proposed in the question. I think that more details are worthed.
The key ingredient for that definition is the concept of arrow category of a given category $\mathbf D$: such category have morphism of $\mathbf D$ as objects and commutative square as morphisms.
This category come equipped with two functors $\mathbf {source}, \mathbf{target} \colon \text{Arr}(\mathbf D) \to \mathbf D$ such that for each object (i.e. a morphisms of $\mathbf D$) $f \colon d \to d'$ we have $$\mathbf{source}(f)=d$$ $$\mathbf{target}(f)=d'$$ while for each $f \in \mathbf D(x,x')$, $g \in \mathbf D(y,y')$ and a morphism $\alpha \in \text{Arr}(\mathbf D)(f,g)$ (i.e. a quadruple $\langle f,g, \alpha_0,\alpha_1\rangle$ where $\alpha_0 \in \mathbf D(x,y)$ and $\alpha_1 \in \mathbf D(x',y')$ such that $\alpha_1 \circ f = g \circ \alpha_0$) we have $$\mathbf{source}(\alpha)=\alpha_0$$ $$\mathbf{target}(\alpha)=\alpha_1$$ it's easy to prove that these data give two functors (which gives to $\text{Arr}(\mathbf D)$ the structure of a graph internal to $\mathbf{Cat}$).
Now let's take a look to this new definition of natural transformation:
A natural transformation $\tau$ between two functors $F,G \colon \mathbf C \to \mathbf D$ is a functor $\tau \colon \mathbf C \to \text{Arr}(\mathbf D)$ such that $\mathbf{source} \circ \tau = F$ and $\mathbf{target}\circ \tau = G$.
A functor of this kind associate to every object $c \in \mathbf C$ a morphism $\tau_c \colon F(c) \to G(c)$ in $\mathbf D$, while to every $f \in \mathbf C(c,c')$ it gives the commutative triangle expressing the equality $$\tau_{c'} \circ F(f)=\tau_{c'} \circ \mathbf {source}(\tau_f)=\mathbf {target}(\tau_f) \circ \tau_c = G(f) \circ \tau_c$$ certifying the naturality (in the ordinary sense) of the $\tau_c$. This definition reminds the notion of homotopy between maps $f,g \colon X \to Y$ as map of kind $X \to Y^I$ (i.e. an homotopy as a (continuous) family of path of $Y$).
That's not all, indeed we can reiterate the construction of the arrow category obtaining what I think is called a cubical set $$\mathbf D \leftarrow \text{Arr}(\mathbf D) \leftarrow \text{Arr}^2(\mathbf D)\leftarrow \dots $$ where each arrow should be thought as the pair of functors $\mathbf{source}_{n+1},\mathbf{target}_{n+1} \colon \text{Arr}^{n+1}(\mathbf D) \to \text{Arr}^n (\mathbf D)$.
In this way we can associate to each category a cubical set. There's also a natural way to associate to every functor a (degree 0) mapping of cubical sets.
If we consider natural transformation as maps from a category to an arrow category then this correspondence associate to each natural transformation a degree 1 map between such cubical sets (by degree one I mean that the induced map send every object of $\text{Arr}^n(\mathbf C)$ in an object of $\text{Arr}^{n+1}(\mathbf D)$). I've found really beautiful this construction because it shows an analogy between categories-functors-natural transformation and complexes-map of complexes-complexes homotopies.