To show that $ZFC$ is not existentially closed, we can use the following forcing argument: Let the ground model can model $V=L$ and the forcing extension model $2^{{\aleph}_{0}}=\aleph_{2}$. (Maybe there is a simpler proof of this fact, but I can't see it right now).
However suppose that I were to refine my question. Suppose that $ZFC\subseteq{T}$ is complete and consistent. Is $T$ existentially closed? If I were to guess, I would guess no. However I'm having trouble proving this.
I would guess the same for a complete theory $Th({\mathbb{N}},+, \times, <,0,1) \subseteq{T'}$, and I would like to have an argument that is applicable in both cases.
My original idea for both was to exploit the fact that for an infinite linear order where each element has a unique predecessor and a unique successor, I can show that a structure is not existentially closed by adding an element in between two elements to obtain an extension. However this idea fails for $Th({\mathbb{N}},+, \times, <,0,1)$ in the following sense:
Given $M\models{T'}$ and $a,b\in{M}$ such that $b=a+1$, I can't use compactness to add a new $c$ s.t. $a<c<b$ while also extending $T'\cup{\text{Diag}(M)}$ for the following reason; as $b=a+1$ will be in the diagram of $M$ that I'm trying to extend and $a<c<b$ would imply $b\neq{a+1}$ in the extension. So the option seems to be to construct models witnessing the failure of the criterion from scratch.
I'm not sure about $ZFC\subseteq{T}$. There will be a lot of linear orders (without any additional structure as in the above example) in a model of $T$ to play around with, but extending a model of set theory is not an easy task!
Edit: Or is my guess wrong and are models of the theories I'm interested in existentially closed (and hence model complete)?. I would be surprised by such a result as extensions of $ZFC$ tend to be badly behaved.