Per your comment, if the subgroups are unique you can do
library(dplyr)
group_by(df, group) %>% mutate(percent = value/sum(value))
# group subgroup value percent
# 1 A a 1 0.1250000
# 2 A b 4 0.5000000
# 3 A c 2 0.2500000
# 4 A d 1 0.1250000
# 5 B a 1 0.1666667
# 6 B b 2 0.3333333
# 7 B c 3 0.5000000
Or to remove the value
column and add the percent
column at the same time, use transmute
group_by(df, group) %>% transmute(subgroup, percent = value/sum(value))
# group subgroup percent
# 1 A a 0.1250000
# 2 A b 0.5000000
# 3 A c 0.2500000
# 4 A d 0.1250000
# 5 B a 0.1666667
# 6 B b 0.3333333
# 7 B c 0.5000000