It's ugly, but does the job. It breaks up the rcases environment content, so that an alignment point can be added around the equals sign. That, in and of itself causes issues that have to be remedied with the nonstandard use of ={}& rather than &=, as well as the addition of \mkern-5mu to undo rcases horizontal padding.
However, in addition, a magic \vphantom has to be added to get the aligned to the left side of the equation to have the same vertical spacing as the rcases on the right side.
EDITED to take Mico's suggestion of removing the excessive \left...\right syntax, and of using the bm package.
\documentclass{article} \usepackage{amsmath,mathtools,bm} \usepackage[margin=2.5cm]{geometry} \begin{document} \begin{equation} \begin{split} \bm{d}^{(0)} ={}& 0 \\ \bm{\phi}^{( 0)} ={}& \bm{\phi}^k \\ \begin{aligned} \bm{d}^{(m)} ={}\\ \bm{\phi}^{(m)} ={}\vphantom{\Bigl(} \end{aligned} & \mkern-5mu\begin{rcases} \beta_m \bm{D}\bm{\phi}^{(m-1)} + ( 1 - \beta_m) \bm{d}^{( m-1)} \\ \bm{\phi}^{(0)} + a_m \mathcal{P} \Bigl( \bm{f} - \bm{C} \phi^{(m-1)} - \bm{d}^{(m)} - V\frac{3\bm{\phi}_n^{(m-1)}-4\bm{\phi}_{n-1}+\bm{\phi}_{n-2}}{2\Delta t}\Bigr) \end{rcases} m =1,2,\dots, 5 \\ \bm{\phi}^{k+1} ={}& \bm{\phi}^{(5)} \end{split} \end{equation} \end{document}

ORIGINAL ANSWER (for comparison))
\documentclass{article} \usepackage{amsmath,mathtools} \usepackage[margin=2.5cm]{geometry} \begin{document} \begin{align} \begin{split} \boldsymbol{d}^{\left( 0\right)} ={}& 0 \\ \boldsymbol{\phi}^{\left( 0\right)} ={}& \boldsymbol{\phi}^k \\ \begin{aligned} \boldsymbol{d}^{\left( m\right)} ={}\\ \boldsymbol{\phi}^{\left( m\right)} ={}\vphantom{\left(\textstyle\frac{x_{n-1}^{(}}{}\right)} \end{aligned} & \mkern-5mu\begin{rcases} \beta_m \boldsymbol{D}\boldsymbol{\phi}^{\left(m-1\right)} + \left( 1 - \beta_m \right) \boldsymbol{d}^{\left( m-1\right)} \\ \boldsymbol{\phi}^{\left( 0\right)} + a_m \mathcal{P} \left( \boldsymbol{f} - \boldsymbol{C} \phi^{\left( m-1\right)} - \boldsymbol{d}^{\left( m\right)} - V\frac{3\boldsymbol{\phi}_n^{\left( m-1\right)}-4\boldsymbol{\phi}_{n-1}+\boldsymbol{\phi}_{n-2}}{2\Delta t}\right) \end{rcases} m =1,2,\dots, 5 \\ \boldsymbol{\phi}^{k+1} ={}& \boldsymbol{\phi}^{\left( 5\right)} \end{split} \end{align} \end{document}

\documentclassand ending with\end{document}. (this expression is too wide forarticle, so you must be using something else.) also, not material to the question, instead of the combination ofalignandsplit, a more "conventional" combination would beequationandaligned, although it doesn't improve the alignment.