The aggregate expression for sorting needs to be on the individual item's Group and not on the dataset, table or chart's properties.
You may be getting a silent error that lets the report run but fails to evaluate the expression due to a possible divide by zero issue. If you preview the report in Visual Studio, you may see the error in the Error List.
SSRS like to be smart and check for possible issues with dividing by zero. Unfortunately, it finds any place that a field could be zero. To get around this, use IIF statements so that it replaces the possible zero divisor with a 1 and the numerator with a zero. Your expression is a bit more complicate since you have two divisors but it should be something like
= IIF(Sum(Fields!Marketvalue.Value + Fields!AccruedInterest.Value) = 0
OR Fields!EquityTarget.Value = 0,
0,
SUM(IIF(Fields!SecTypeBaseCode.Value="cs", Fields!Marketvalue.Value, 0))
)
/
IIF(Sum(Fields!Marketvalue.Value + Fields!AccruedInterest.Value) = 0,
1,
Sum(Fields!Marketvalue.Value + Fields!AccruedInterest.Value))
/
IIF(Fields!EquityTarget.Value = 0, 1, Fields!EquityTarget.Value)
*
100
See also:
Avoid divide by zero in SSRS expression
SSRS Expression Divide by Zero Error
Attemted to divide by zero error in SSRS Expression